REFERENCES
1. Park, S.; Heo, S. W.; Lee, W.; et al. Self-powered ultra-flexible electronics via nano-grating-patterned organic photovoltaics. Nature 2018, 561, 516-21.
2. Jing, Z.; Sun, A.; He, Z.; et al. Highly robust and conductive polymer electrodes for droplet energy harvesting and printable on-skin electronics. Adv. Mater. 2025, 37, 2506511.
3. Meng, S.; Zhao, T.; Wang, X.; Wang, X.; Zhang, Y. High-dielectric PVDF/MXene composite dielectric materials for energy storage preparation and performance study. Polym. Compos. 2023, 45, 3460-73.
4. Li, Z.; Zhao, K.; Wang, J.; et al. Sensitive, robust, wide-range, and high-consistency capacitive tactile sensors with ordered porous dielectric microstructures. ACS. Appl. Mater. Interfaces. 2024, 16, 7384-98.
5. Zhao, S.; Liu, H. Y.; Cui, L.; et al. Elastomeric nanodielectrics for soft and hysteresis-free electronics. Adv. Mater. 2021, 33, 2104761.
6. Li, Y.; Zhai, W.; Liu, B.; et al. Remarkable interfacial dielectric relaxation of physically cross-linked ice-hydrogel. Soft. Sci. 2021, 1, 11.
7. Xing, J.; Yi, X.; Qu, Y.; et al. Helical ionotropic gel-fiber sensor with omnidirectional strain perception for multidimensional motion correction in adolescent activity assessment. Soft. Sci. 2025, 5, 37.
8. Crawford, K. E.; Sita, L. R. De novo design of a new class of “hard-soft” amorphous, microphase-separated, polyolefin block copolymer thermoplastic elastomers. ACS. Macro. Lett. 2015, 4, 921-5.
9. Munzenrieder, N.; Voser, P.; Petti, L.; et al. Flexible self-aligned double-gate IGZO TFT. IEEE. Electron. Device. Lett. 2014, 35, 69-71.
10. Zou, S.; Picella, S.; de Vries, J.; Kortman, V. G.; Sakes, A.; Overvelde, J. T. B. A retrofit sensing strategy for soft fluidic robots. Nat. Commun. 2024, 15, 539.
11. Fan, Z.; Dai, J.; Huang, Y.; et al. Superior energy storage capacity of polymer-based bilayer composites by introducing 2D ferroelectric micro-sheets. Nat. Commun. 2025, 16, 1180.
12. Qiu, Y.; Zhang, E.; Plamthottam, R.; Pei, Q. Dielectric elastomer artificial muscle: materials innovations and device explorations. Acc. Chem. Res. 2019, 52, 316-25.
13. Benouhiba, A.; Holzer, S.; Konstantinidi, S.; Civet, Y.; Perriard, Y. The elastic frontier: dielectric elastomer actuators in healthcare technology. Smart. Mater. Struct. 2025, 34, 033001.
14. Cheng, N.; Liu, C.; Gao, Y.; et al. Ultra-elastic, durable, bio-degradable, and recyclable pulp foam as an air dielectric substitute for sustainable capacitive pressure sensing. Adv. Funct. Mater. 2025, 35, 2423122.
15. Shu, L.; Liang, R.; Yu, Y.; Tian, T.; Rao, Z.; Wang, Y. Unique elastic, dielectric and piezoelectric properties of micro-architected metamaterials. J. Mater. Chem. C. 2019, 7, 2758-65.
16. Zeng, T.; Meng, L.; Li, Q.; et al. Enhancing energetic disorder in all-organic composite dielectrics for high-temperature capacitive energy storage. Nat. Commun. 2025, 16, 5620.
17. Qian, X.; Chen, X.; Zhu, L.; Zhang, Q. M. Fluoropolymer ferroelectrics: multifunctional platform for polar-structured energy conversion. Science 2023, 380, eadg0902.
18. Wang, L.; Zhuo, J.; Peng, J.; Dong, H.; Jiang, S.; Shi, Y. A stretchable soft pump driven by a heterogeneous dielectric elastomer actuator. Adv. Funct. Mater. 2024, 34, 2411160.
19. Gao, L.; Hu, B. L.; Wang, L.; et al. Intrinsically elastic polymer ferroelectric by precise slight cross-linking. Science 2023, 381, 540-4.
20. Kim, J.; Zhang, G.; Shi, M.; Suo, Z. Fracture, fatigue, and friction of polymers in which entanglements greatly outnumber cross-links. Science 2021, 374, 212-6.
21. Pan, C.; Markvicka, E. J.; Malakooti, M. H.; et al. A liquid-metal-elastomer nanocomposite for stretchable dielectric materials. Adv. Mater. 2019, 31, 1900663.
22. Yin, L. J.; Zhao, Y.; Zhu, J.; et al. Soft, tough, and fast polyacrylate dielectric elastomer for non-magnetic motor. Nat. Commun. 2021, 12, 4517.
23. Liu, Y.; Yue, S.; Tian, Z.; et al. Self-powered and self-healable extraocular-muscle-like actuator based on dielectric elastomer actuator and triboelectric nanogenerator. Adv. Mater. 2024, 36, 2309893.
24. Wang, Y.; Cui, J.; Yuan, Q.; Niu, Y.; Bai, Y.; Wang, H. Significantly enhanced breakdown strength and energy density in sandwich-structured barium titanate/poly(vinylidene fluoride) nanocomposites. Adv. Mater. 2015, 27, 6658-63.
25. Lang, C.; Lloyd, E. C.; Matuszewski, K. E.; et al. Nanostructured block copolymer muscles. Nat. Nanotechnol. 2022, 17, 752-8.
26. Wang, S.; Yang, C.; Li, X.; et al. Polymer-based dielectrics with high permittivity and low dielectric loss for flexible electronics. J. Mater. Chem. C. 2022, 10, 6196-221.
27. Yue, D.; Yin, J. H.; Zhang, W. C.; et al. Computational simulation for breakdown and energy storage performances with optimization in polymer dielectrics. Adv. Funct. Mater. 2023, 33, 2300658.
28. Yin, G.; Yang, Y.; Song, F.; et al. Dielectric elastomer generator with improved energy density and conversion efficiency based on polyurethane composites. ACS. Appl. Mater. Interfaces. 2017, 9, 5237-43.
29. Bonardd, S.; Moreno-Serna, V.; Kortaberria, G.; Díaz, Díaz. D.; Leiva, A.; Saldías, C. Dipolar glass polymers containing polarizable groups as dielectric materials for energy storage applications. A minireview. Polymers 2019, 11, 317.
30. Li, F.; Gao, L.; Wang, L.; Hu, B. Unlocking the elasticity in ferroelectrics by slight crosslinking. Chin. J. Struct. Chem. 2025, 44, 100443.
31. Feng, Q. K.; Zhong, S. L.; Pei, J. Y.; et al. Recent progress and future prospects on all-organic polymer dielectrics for energy storage capacitors. Chem. Rev. 2022, 122, 3820-78.
32. Hu, Q.; Wang, L.; Pan, L.; Hu, B. L. Slight-crosslinking: opening a new journey for the intrinsic elastification of ferroelectric polymers. Chemistry 2025, 31, e202500247.
33. Alhasadi, M. F.; Sun, Q.; Federico, S. Theory of uniformity applied to elastic dielectric materials and piezoelectricity. Eur. J. Mech. A. Solids. 2022, 91, 104391.
34. Liu, L.; Qu, J.; Gu, A.; Wang, B. Percolative polymer composites for dielectric capacitors: a brief history, materials, and multilayer interface design. J. Mater. Chem. A. 2020, 8, 18515-37.
35. Dakin, T. Conduction and polarization mechanisms and trends in dielectric. IEEE. Electr. Insul. Mag. 2006, 22, 11-28.
36. Prateek, Thakur, V.K.; Gupta, R.K. Recent progress on ferroelectric polymer-based nanocomposites for high energy density capacitors: synthesis, dielectric properties, and future aspects. Chem. Rev. 2016, 116, 4260-317.
37. Yadegari, A.; Ebel, T. Exploring modification strategies to enhance energy storage performance of BOPP dielectric films. J. Mater. Chem. A. 2025, 13, 30768-95.
38. Wang, B.; Liang, G.; Jiao, Y.; et al. Two-layer materials of polyethylene and a carbon nanotube/cyanate ester composite with high dielectric constant and extremely low dielectric loss. Carbon 2013, 54, 224-33.
39. Yang, M.; Ren, W.; Guo, M.; Shen, Y. High-energy-density and high efficiency polymer dielectrics for high temperature electrostatic energy storage: a review. Small 2022, 18, 2205247.
40. Qin, M.; Zhang, L.; Wu, H. Dielectric loss mechanism in electromagnetic wave absorbing materials. Adv. Sci. 2022, 9, 2105553.
41. Tian, G.; Deng, W.; Yang, T.; et al. Insight into interfacial polarization for enhancing piezoelectricity in ferroelectric nanocomposites. Small 2023, 19, 2207947.
42. Wei, J.; Zhu, L. Intrinsic polymer dielectrics for high energy density and low loss electric energy storage. Prog. Polym. Sci. 2020, 106, 101254.
43. Rui, G.; Bernholc, J. J.; Zhang, S.; Zhang, Q. Dilute nanocomposites: tuning polymer chain local nanostructures to enhance dielectric responses. Adv. Mater. 2024, 36, 2311739.
44. Deng, Y.; Zhang, Q.; Qu, D. Emerging hydrogen-bond design for high-performance dynamic polymeric materials. ACS. Mater. Lett. 2023, 5, 480-90.
45. Chen, L.; Liu, Y.; You, W.; et al. Construction of slide-ring polymers based on pillar[5]arene/alkyl chain host-guest interactions. Angew. Chem. Int. Ed. 2025, 64, e202417713.
46. Kim, M.; Park, H.; Kim, E.; Chung, M.; Oh, J. H. Photo-crosslinkable organic materials for flexible and stretchable electronics. Mater. Horiz. 2025, 12, 4573-607.
47. Kong, V. A.; Staunton, T. A.; Laaser, J. E. Effect of cross-link homogeneity on the high-strain behavior of elastic polymer networks. Macromolecules 2024, 57, 4670-9.
48. Deng, J.; Bai, R.; Zhao, J.; et al. Insights into the correlation of cross-linking modes with mechanical properties for dynamic polymeric networks. Angew. Chem. Int. Ed. 2023, 62, e202309058.
49. Zhao, S.; Zhang, Z.; Yin, L.; et al. CPBA/PVDF dielectric elastomer composites with high actuation performance under low electric field by optimizing the internal structure. Polymer 2025, 336, 128867.
50. Park, C.; Lee, K.; Koo, M.; Park, C. Soft ferroelectrics enabling high-performance intelligent photo electronics. Adv. Mater. 2021, 33, e2004999.
51. Raji, I. O.; Dodo, O. J.; Saha, N. K.; et al. Network polymer properties engineered through polymer backbone dispersity and structure. Angew. Chem. Int. Ed. 2024, 63, e202315200.
52. Zhang, W.; Xiong, T.; Bai, Z.; Liu, H.; Qiu, X. Solid-state electrolytes based on polyimides for lithium batteries: structures, key properties, synthesis methods and applications. Electrochem. Energy. Rev. 2025, 8, 33.
53. Chen, P.; Wang, H.; Su, J.; et al. Recent advances on high-performance polyaryletherketone materials for additive manufacturing. Adv. Mater. 2022, 34, 2270360.
54. Wu, C.; Deshmukh, A. A.; Li, Z.; et al. Molecular engineering: flexible temperature-invariant polymer dielectrics with large bandgap. Adv. Mater. 2020, 32, 2070165.
55. Xiao, Y.; Chen, Z.; Mao, J.; et al. Self-strengthening dielectric elastomer of triblock copolymer with significantly improved electromechanical performance under low voltage. Macromol. Mater. Eng. 2021, 306, 2000732.
56. He, G.; Liu, Z.; Wang, C.; Chen, S.; Luo, H.; Zhang, D. Achieving superior energy storage properties of all-organic dielectric polystyrene-based composites by blending rod-coil block copolymers. ACS. Sustainable. Chem. Eng. 2021, 9, 8156-69.
57. de Sousa Jr, R. R.; Sacramento, J. B.; Da Silva, L. C. E.; Becker, D.; Vidotti, S. E.; Carastan, D. J. High-performance block-copolymer-based dielectric elastomers with enhanced mechanical properties. ACS. Appl. Polym. Mater. 2023, 5, 9505-14.
58. Liu, Y.; Chen, J.; Jiang, X.; Jiang, P.; Huang, X. All-organic cross-linked polysiloxane-aromatic thiourea dielectric films for electrical energy storage application. ACS. Appl. Energy. Mater. 2020, 3, 5198-207.
59. Yang, D.; Tian, M.; Kang, H.; et al. New polyester dielectric elastomer with large actuated strain at low electric field. Mater. Lett. 2012, 76, 229-32.
60. Luo, H.; Yan, C.; Liu, X.; Luo, H.; Chen, S. Constructing novel high-performance dipolar glass polymer dielectrics by polar rigid/flexible side chains. ACS. Appl. Mater. Interfaces. 2023, 15, 24470-82.
61. Gao, L.; Zhang, J.; Wang, L.; et al. Highly elastic relaxor ferroelectrics for wearable energy storage. Mater. Horiz. 2024, 11, 6150-7.
62. Xu, T.; Wang, L.; Gao, L.; et al. Intrinsic elastomer with remarkable dielectric constant via elastification of relaxor ferroelectric polymer. Adv. Mater. 2024, 36, 2404001.
63. Panyukov, S. Theory of flexible polymer networks: elasticity and heterogeneities. Polymers 2020, 12, 767.
65. Fan, Y.; Shen, Z.; Zhou, X.; et al. Highly sensitive strain sensor from topological-structure modulated dielectric elastic nanocomposites. Adv. Mater. Technol. 2021, 7, 2101190.
66. Sun, H.; Kabb, C. P.; Sims, M. B.; Sumerlin, B. S. Architecture-transformable polymers: reshaping the future of stimuli-responsive polymers. Prog. Polym. Sci. 2019, 89, 61-75.
67. Li, L.; Xu, W.; Rui, G.; Zhang, S.; Zhang, Q. M.; Wang, Q. Dilute nanocomposites for capacitive energy storage: progress, challenges and prospects. Chem. Sci. 2024, 15, 19651-68.
68. Xie, Z.; Liu, D.; Xiao, Y.; et al. The effect of filler permittivity on the dielectric properties of polymer-based composites. Compos. Sci. Technol. 2022, 222, 109342.
69. Huang, X.; Sun, B.; Zhu, Y.; Li, S.; Jiang, P. High-k polymer nanocomposites with 1D filler for dielectric and energy storage applications. Prog. Mater. Sci. 2019, 100, 187-225.
70. Han, Y.; Zhang, Y.; Huang, P.; et al. A dielectric elastomer containing bicomponent core-shell nanoparticles with enhanced electromechanical properties for flexible crawling Robots. ACS. Appl. Polym. Mater. 2024, 6, 6667-78.
71. Zhang, J.; Zhao, F.; Zuo, Y.; et al. Improving actuation strain and breakdown strength of dielectric elastomers using core-shell structured CNT-Al2O3. Compos. Sci. Technol. 2020, 200, 108393.
72. Huang, B.; Yu, Y.; Zhao, Y.; et al. Al@SiO2 core-shell fillers enhance dielectric properties of silicone composites. ACS. Omega. 2023, 8, 35275-82.
73. Sun, H.; Zhang, T.; Sun, H.; et al. Improved the high-temperature energy storage performance of PEI films via loading core-shell structured Al2O3@BaSrTiO3 nanofillers. Ceram. Int. 2024, 50, 43811-8.
74. Zhou, W.; Cao, G.; Yuan, M.; et al. Core-shell engineering of conductive fillers toward enhanced dielectric properties: a universal polarization mechanism in polymer conductor composites. Adv. Mater. 2023, 35, 2207829.
75. Hussain, A.; Luo, S.; Jawaid, J.; et al. Interface-engineered core-shell nanoparticle embedded polymer nanocomposite demonstrating low voltage and temperature dependent tunable dielectric response. J. Mater. Chem. A. 2025, 13, 30587-98.
76. Guo, Y.; Liu, S.; Wu, S.; et al. Enhanced tunable dielectric properties of Ba0.6Sr0.4TiO3/PVDF composites through dual-gradient structural engineering. J. Alloys. Compd. 2022, 920, 166034.
77. Wang, P.; Guo, Z.; Sun, Z.; Li, G.; Bi, J.; Qian, L. Carrier gradient core-double shell structure with heterojunction transition layer for significantly enhancing dielectric properties. Chem. Eng. J. 2024, 496, 153968.
78. Wu, W.; Liu, X.; Qiang, Z.; et al. Inserting insulating barriers into conductive particle channels: a new paradigm for fabricating polymer composites with high dielectric permittivity and low dielectric loss. Compos. Sci. Technol. 2021, 216, 109070.
79. Guo, R.; Luo, H.; Zhai, D.; et al. Ultrahigh energy density in dielectric nanocomposites by modulating nanofiller orientation and polymer crystallization behavior. Adv. Powder. Mater. 2024, 3, 100212.
80. Pabba, D. P.; Rao, B. B.; Thiam, A.; et al. Magnetic field assisted high performance triboelectric nanogenerators based on P(VDF-HFP)/NiFe2O4 nanofiber composite. Ceram. Int. 2024, 50, 4178-89.
81. Li, Z.; An, L.; Khuje, S.; et al. Solution-shearing of dielectric polymer with high thermal conductivity and electric insulation. Sci. Adv. 2021, 7, eabi7410.
82. Wang, L.; Luo, H.; Zhou, X.; Yuan, X.; Zhou, K.; Zhang, D. Sandwich-structured all-organic composites with high breakdown strength and high dielectric constant for film capacitor. Compos. Part. A. Appl. Sci. Manuf. 2019, 117, 369-76.
83. Shi, Y.; Askounis, E.; Plamthottam, R.; et al. A processable, high-performance dielectric elastomer and multilayering process. Science 2022, 377, 228-32.
84. Su, Y.; Sui, G.; Lan, J.; Yang, X. A highly stretchable dielectric elastomer based on core-shell structured soft polymer-coated liquid-metal nanofillers. Chem. Commun. 2020, 56, 11625-8.
85. Tang, C.; Han, B.; Dong, L.; et al. In-situ confined transformation of Ti3C2Tx in electrospun SiC fiber matrix for optimized conductive loss and polarization loss. Chem. Eng. J. 2025, 521, 166507.
86. Zhang, L.; Zhang, S.; Wang, C.; Zhou, Q.; Zhang, H.; Pan, G. B. Highly sensitive capacitive flexible pressure sensor based on a high-permittivity MXene nanocomposite and 3D network electrode for wearable electronics. ACS. Sens. 2021, 6, 2630-41.
87. Chen, Y.; Huang, Z.; Hu, F.; et al. Microstructured polyfluoroacrylate elastomeric dielectric layer for highly stretchable wide-range capacitive pressure sensors. ACS. Appl. Mater. Interfaces. 2023, 15, 58700-10.
88. Feng, Z. P.; Hao, Y. N.; Qin, J.; et al. Ultrasmall barium titanate nanoparticles modulated stretchable dielectric elastomer sensors with large deformability and high sensitivity. InfoMat 2023, 5, e12413.
89. Peng, J.; Zhuo, J.; Dong, H.; et al. Dielectric elastomer actuators with low driving voltages and high mechanical outputs enabled by a scalable ultra-thin film multilayering process. Adv. Funct. Mater. 2024, 34, 2411801.
90. Huang, J.; Zhang, X.; Liu, R.; Ding, Y.; Guo, D. Polyvinyl chloride-based dielectric elastomer with high permittivity and low viscoelasticity for actuation and sensing. Nat. Commun. 2023, 14, 1483.
91. Shi, L.; Yang, R.; Lu, S.; et al. Dielectric gels with ultra-high dielectric constant, low elastic modulus, and excellent transparency. NPG. Asia. Mater. 2018, 10, 821-6.
92. Tang, T.; Yang, W.; Shen, Z.; et al. Compressible polymer composites with enhanced dielectric temperature stability. Adv. Mater. 2023, 35, 2209958.
93. Li, T.; Yi, S.; Sun, W.; et al. Constructing fluorinated triphenyl in carbonate copolymers toward flexible high energy-storable dielectric films with enhanced thermal resistance. Nano. Energy. 2024, 130, 110105.
94. Kim, S. H.; Basir, A.; Avila, R.; et al. Strain-invariant stretchable radio-frequency electronics. Nature 2024, 629, 1047-54.
95. Hu, W.; Ren, Z.; Li, J.; Askounis, E.; Xie, Z.; Pei, Q. New dielectric elastomers with variable moduli. Adv. Funct. Mater. 2015, 25, 4827-36.
96. Hu, J.; Sun, M.; Wei, T.; Chen, C.; Wan, X.; Mu, Y. Low-voltage organic field-effect transistors using a phosphocholine-based polyampholyte dielectric. Macromolecules 2025, 58, 5618-26.
97. Sun, Q.; Hu, J.; Chen, C.; Wan, X.; Mu, Y. Functional zwitterionic polyurethanes as gate dielectrics for organic field-effect transistors. Adv. Elect. Mater. 2024, 11, 2400578.
98. Li, W.; Wu, S.; Zhou, Q.; Gong, C.; Liu, Z.; Yan, Y. Harmonizing elastic modulus and dielectric constant of elastomers for improved pressure sensing performance. ACS. Appl. Mater. Interfaces. 2024, 16, 32727-38.
99. He, J.; Chen, Z.; Xiao, Y.; et al. Intrinsically anisotropic dielectric elastomer fiber actuators. ACS. Materials. Lett. 2022, 4, 472-9.
100. Yang, L.; Wang, H. High-performance electrically responsive artificial muscle materials for soft robot actuation. Acta. Biomater. 2024, 185, 24-40.
101. Wang, R.; Liang, Y.; Xiao, J.; et al. Multilayer assembly of dielectric actuators based on a reversibly crosslinkable silicone elastomer. Adv. Funct. Mater. 2025, 36, e09974.
102. Zhang, Y.; Song, Z.; Yu, W.; et al. Dielectric elastomer with covalently charged interpenetrated polyacrylate network for large actuation strain under low driving electric field. Chem. Eng. J. 2025, 520, 165877.
103. Shu, L.; Shi, X.; Zhang, X.; et al. Partitioning polar-slush strategy in relaxors leads to large energy-storage capability. Science 2024, 385, 204-9.
104. Zhang, T.; Sun, H.; Yin, C.; et al. Recent progress in polymer dielectric energy storage: from film fabrication and modification to capacitor performance and application. Prog. Mater. Sci. 2023, 140, 101207.
105. Cao, Z.; Xu, X.; Sun, F.; et al. Depolymerizable thermosetting dielectric elastomers toughened by sacrificial hydrogen bonds for sustainable capacitive strain-sensor. Adv. Funct. Mater. 2025, 35, 2505979.
106. Jiang, Y.; Liu, X.; Wang, Y.; et al. High energy harvesting performances silicone elastomer via filling soft dielectric with stretching deformability. Adv. Mater. 2023, 35, 2300246.
107. Wang, Z.; Tang, C.; Wang, Y.; et al. Enhancing the energy conversion efficiency of dielectric elastomer generators via elastic energy storage and recovery. Appl. Energy. 2025, 379, 124854.
108. Duan, L.; Lai, J. C.; Li, C. H.; Zuo, J. L. A dielectric elastomer actuator that can self-heal integrally. ACS. Appl. Mater. Interfaces. 2020, 12, 44137-46.
109. Yang, D.; Zhao, K.; Yang, R.; et al. A rational design of bio-derived disulfide CANs for wearable capacitive pressure sensor. Adv. Mater. 2024, 36, 2403880.
110. Madsen, F. B.; Yu, L.; Skov, A. L. Self-healing, high-permittivity silicone dielectric elastomer. ACS. Macro. Lett. 2016, 5, 1196-200.
111. Zhang, Y.; Ellingford, C.; Zhang, R.; et al. Electrical and mechanical self-healing in high-performance dielectric elastomer actuator materials. Adv. Funct. Mater. 2019, 29, 1808431.
112. Huang, B.; Yu, Y.; Zhao, Y.; et al. Efficient self-repairing high permittivity cyanosilicone dielectric elastomers. Polymer 2023, 280, 126047.
113. Tan, M. W. M.; Thangavel, G.; Lee, P. S. Rugged soft robots using tough, stretchable, and self-healable adhesive elastomers. Adv. Funct. Mater. 2021, 31, 2103097.
