Microphase-Separated Liquid Crystal Elastomer Actuators With Exceptional Strength and Toughness

Abstract

Liquid crystal elastomers (LCEs) have emerged as attractive soft actuators capable of undergoing large and reversible actuation. Their potential for practical applications, however, has been fundamentally constrained by an intrinsic trade-off: the chain flexibility required for reversible actuation inherently restricts molecular design toward achieving high mechanical strength and toughness. Here, we report a phase separation strategy that yields an LCE with a tensile strength of 92 MPa and toughness of 247 MJ m⁻³. This leads to 20-fold and 40-fold improvements compared with conventional LCEs without sacrificing their reversible actuation. Mechanistically, this superior mechanical performance is enabled by the incorporation of rigid polyamide acid segments into the network. During network formation, these segments self-assemble into phase-separated nanostructures that function as in situ-generated nanofillers, reinforcing the material and endowing it with outstanding work capacity. Our work suggests that leveraging microphase separation substantially broadens the design space for high-performance LCE actuators, paving the way toward mechanically robust and efficient soft actuation systems.

Keywords

liquid crystal elastomers / mechanical properties / microphase separation

References

[1] R. O. Ritchie, “The Conflicts Between Strength and Toughness,” Nature Materials 10 (2011): 817–822.

[2] X. Liao, M. Dulle, J. M. de Souza e Silva, et al., “High Strength in Combination With High Toughness in Robust and Sustainable Polymeric Materials,” Science 366 (2019): 1376–1379.

[3] X. F. Chen, J. Hu, J. X. Huang, et al., “Strong and Tough Single-Network Elastomers Enabled by a Rigid, High-Threshold Nonscissile Mechanophore-Activated Chain Extender,” CCS Chemistry (2026), https://doi.org/10.31635/ccschem.026.202507036.

[4] X. Liu, X. Zhou, and Z. Liu, “Strengthening Liquid Crystal Elastomer Muscles,” Accounts of Chemical Research 58 (2025): 907–918.

[5] L. Liu, M. H. Liu, L. L. Deng, B. P. Lin, and H. Yang, “Near-Infrared Chromophore Functionalized Soft Actuator With Ultrafast Photoresponsive Speed and Superior Mechanical Property,” Journal of the American Chemical Society 139 (2017): 11333–11336.

[6] Z. Jiang, B. B. A. Abbasi, S. Aloko, F. Mokhtari, and G. M. Spinks, “Ultra-Soft Organogel Artificial Muscles Exhibiting High Power Density, Large Stroke, Fast Response and Long-Term Durability in Air,” Advanced Materials 35 (2023): 2210419.

[7] T. J. White and D. J. Broer, “Programmable and Adaptive Mechanics With Liquid Crystal Polymer Networks and Elastomers,” Nature Materials 14 (2015): 1087–1098.

[8] C. Chen, H. Yu, T. Lai, et al., “Flexible and Elastic Thermal Regulator for Multimode Intelligent Temperature Control,” SusMat 3 (2023): 843–858.

[9] H. Guo, C. Liang, T. P. Ruoko, et al., “Programmable and Self-Healable Liquid Crystal Elastomer Actuators Based on Halogen Bonding,” Angewandte Chemie International Edition 62 (2023): e202309402.

[10] T. Zang, S. Fu, J. Cheng, et al., “4D Printing of Shape-Morphing Liquid Crystal Elastomers,” Chemical and Biological Engineering 1 (2024): 488–515.

[11] X. Zhou, B. Yang, and N. Zheng, “Sequentially Autonomous Rolling of Liquid Crystalline Elastomers With Tunable Actuation Temperatures,” Acta Polymerica Sinica 55 (2024): 614–623.

[12] I. H. Kim, S. Choi, J. Lee, et al., “Human-Muscle-Inspired Single Fibre Actuator With Reversible Percolation,” Nature Nanotechnology 17 (2022): 1198–1205.

[13] J. Liu, Y. Gao, H. Wang, R. Poling-Skutvik, C. O. Osuji, and S. Yang, “Shaping and Locomotion of Soft Robots Using Filament Actuators Made From Liquid Crystal Elastomer–Carbon Nanotube Composites,” Advanced Intelligent Systems 2 (2020): 1900163.

[14] K. M. Herbert, H. E. Fowler, J. M. McCracken, K. R. Schlafmann, J. A. Koch, and T. J. White, “Synthesis and Alignment of Liquid Crystalline Elastomers,” Nature Reviews Materials 7 (2021): 23–38.

[15] X. Zhou, Y. Sheng, G. Chen, et al., “Geometrically Insensitive Deform-and-Go Liquid Crystal Elastomer Actuators Through Controlled Radical Diffusion,” Nature Communications 16 (2025): 7536.

[16] W. Hou, J. Wang, and J. Lv, “Bioinspired Liquid Crystalline Spinning Enables Scalable Fabrication of High-Performing Fibrous Artificial Muscles,” Advanced Materials 35 (2023): 2211800.

[17] Z. Jiang, B. H. Tran, M. A. Jolfaei, B. B. A. Abbasi, and G. M. Spinks, “Crack-Resistant and Tissue-Like Artificial Muscles With Low Temperature Activation and High Power Density,” Advanced Materials 36 (2024): 2402278.

[18] S. Zhang, L. Xu, and Y. Zhao, “Mechanically Robust Liquid Crystal Elastomer Actuator Using Combined Covalent and Topological Sliding-Ring Crosslinking,” Chemical Engineering Journal 527 (2026): 171472.

[19] S. Choi, B. Kim, S. Park, J. H. Seo, and S. Ahn, “Slidable Cross-Linking Effect on Liquid Crystal Elastomers: Enhancement of Toughness, Shape-Memory, and Self-Healing Properties,” ACS Applied Materials & Interfaces 14 (2022): 32486–32496.

[20] T. H. Ware, H. Kim, J. M. Boothby, S. Ramachandran, and C. D. Lee, “Tough, Shape-Changing Materials: Crystallized Liquid Crystal Elastomers,” Macromolecules 50 (2017): 4267–4275.

[21] R. Annapooranan, Y. Wang, and S. Cai, “Highly Durable and Tough Liquid Crystal Elastomers,” ACS Applied Materials & Interfaces 14 (2022): 2006–2014.

[22] Y. Deng, G. Liu, A. Brûlet, et al., “Interpenetrating Liquid Crystal Elastomer and Ionogel as Tunable Electroactive Actuators and Sensors,” Advanced Functional Materials 34 (2024): 2403892.

[23] H. F. Lu, M. Wang, X. M. Chen, B. P. Lin, and H. Yang, “Interpenetrating Liquid-Crystal Polyurethane/Polyacrylate Elastomer With Ultrastrong Mechanical Property,” Journal of the American Chemical Society 141 (2019): 14364–14369.

[24] G. Yang, L. Dong, M. Ren, et al., “Coiled Carbon Nanotube Fibers Sheathed by a Reinforced Liquid Crystal Elastomer for Strong and Programmable Artificial Muscles,” Nano Letters 24 (2024): 9608–9616.

[25] Y. Wang, A. Dang, Z. Zhang, et al., “Repeatable and Reprogrammable Shape Morphing From Photoresponsive Gold Nanorod/Liquid Crystal Elastomers,” Advanced Materials 32 (2020): 2004270.

[26] X. Lin, W. Zou, and E. M. Terentjev, “Double Networks of Liquid-Crystalline Elastomers With Enhanced Mechanical Strength,” Macromolecules 55 (2022): 810–820.

[27] Y. Gao, J. Zhong, X. Lyu, B. Jin, W. Liu, and X. Qiu, “Photothermal-Responsive Lignin-Based Liquid Crystalline Elastomers: Constructing High-Performance Artificial Muscles via a Dual Dynamic Network,” Advanced Functional Materials 36 (2026): e75049.

[28] J. H. Lee, J. Bae, J. H. Hwang, et al., “Robust and Reprocessable Artificial Muscles Based on Liquid Crystal Elastomers With Dynamic Thiourea Bonds,” Advanced Functional Materials 32 (2022): 2110360.

[29] S. Chen, M. Zhang, Q. Li, et al., “Visible Light-Responsive Covalent Adaptable Liquid Crystal Elastomers Enabled by Dynamic Allyl Selenide Bonds,” Macromolecules 56 (2023): 5765–5773.

[30] Y. Wu, D. Pei, F. Wei, et al., “Tough and Photo-Plastic Liquid Crystal Elastomer With a 2-Fold Dynamic Linker for Artificial Muscles,” ACS Applied Materials & Interfaces 15 (2023): 44205–44211.

[31] S. J. D. Lugger, S. J. A. Houben, Y. Foelen, M. G. Debije, A. P. H. J. Schenning, and D. J. Mulder, “Hydrogen-Bonded Supramolecular Liquid Crystal Polymers: Smart Materials With Stimuli-Responsive, Self-Healing, and Recyclable Properties,” Chemical Reviews 122 (2022): 4946–4975.

[32] J. Ding, T. Liu, Y. Li, et al., “Locking Alignment of Liquid Crystal Actuators Using Hydrogen Bonds to Enable Room-Temperature Shape Programmability and Enhanced Work Capacity,” Advanced Functional Materials 35 (2024): 2414510.

[33] S. J. D. Lugger, D. J. Mulder, and A. P. H. J. Schenning, “One-Pot Synthesis of Melt-Processable Supramolecular Soft Actuators,” Angewandte Chemie International Edition 61 (2022): e202115166.

[34] E. He, Y. Wu, H. Liang, et al., “Leveraging Catechol Chemistry to Tackle Toughness–Softness-Work Capacity Tradeoff in Reprogrammable Liquid Crystal Actuators,” Nature Communications 16 (2025): 8782.

[35] R. Liang, H. Yu, L. Wang, and D. Shen, “Light-Guided Dynamic Liquid Crystalline Elastomer Actuators Enabled by Mussel Adhesive Protein Chemistry,” Advanced Functional Materials 33 (2023): 2211914.

[36] C. Li, T. Liu, Y. Li, et al., “Enabling Ultra-High Work Capacity and Scalable Processability of Liquid Crystal Actuators Through Densely Entangled Structures,” Advanced Materials 38 (2025): e13876.

[37] M. J. Ford, M. Palaniswamy, C. Ambulo, T. Ware, and C. Majidi, “Size of Liquid Metal Particles Influences Actuation Properties of a Liquid Crystal Elastomer Composite,” Soft Matter 16 (2020): 5878–5885.

[38] C. Tao, X. Lu, X. Li, and J. Sun, “Robust yet Deformable Nanodomains for Super-Strong and Ultra-Tough Reversibly Cross-Linked Plastics,” National Science Review 12 (2025): nwaf512.

[39] S. H. Choi, J. H. Kim, J. Ahn, et al., “Phase Patterning of Liquid Crystal Elastomers by Laser-Induced Dynamic Crosslinking,” Nature Materials 23 (2024): 834–843.

[40] Y. Yao, A. M. Wilborn, B. Lemaire, et al., “Programming Liquid Crystal Elastomers for Multistep Ambidirectional Deformability,” Science 386 (2024): 1161–1168.

[41] S. Vasanji, M. G. Scarfo, A. Alyami, et al., “Stiffening Liquid Crystal Elastomers With Liquid Crystal Inclusions,” Advanced Materials 37: 2504592.

[42] F. Cai, Y. X. Chen, W. Z. Wang, and H. F. Yu, “Macroscopic Regulation of Hierarchical Nanostructures in Liquid-Crystalline Block Copolymers Towards Functional Materials,” Chinese Journal of Polymer Science 39 (2021): 397–416.

[43] H. Guo, M. O. Saed, and E. M. Terentjev, “Main-Chain Nematic Side-Chain Smectic Composite Liquid Crystalline Elastomers,” Advanced Functional Materials 33 (2023): 2214918.

[44] Z. Guo, X. Lu, X. Wang, X. Li, J. Li, and J. Sun, “Engineering of Chain Rigidity and Hydrogen Bond Cross-Linking Toward Ultra-Strong, Healable, Recyclable, and Water-Resistant Elastomers,” Advanced Materials 35 (2023): 2300286.

[45] Y. Wang, Z. Wang, X. Wang, and J. Sun, “Engineering of Flexible–Rigid Binary Complementary Network Toward Mechanically Robust Elastomers Simultaneously Integrating Extreme Low-Temperature and High-Temperature Resistance,” Macromolecules 58 (2025): 885–896.

[46] D. Liaw, K. Wang, Y. Huang, K. Lee, J. Lai, and C. Ha, “Advanced Polyimide Materials: Syntheses, Physical Properties and Applications,” Progress in Polymer Science 37 (2012): 907–974.

[47] G. Chen, H. Feng, X. Zhou, et al., “Programming Actuation Onset of a Liquid Crystalline Elastomer via Isomerization of Network Topology,” Nature Communications 14 (2023): 6822.

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2026 The Author(s). Aggregate published by SCUT, AIEI, and John Wiley & Sons Australia, Ltd.