Abstract
Natural organisms often couple reversible shape reconfiguration and autonomous motion to adapt and respond to dynamic environments. However, synthetic soft materials rarely achieve both behaviors within a single platform due to fundamental trade-offs in structural anisotropy, solvent compatibility, and actuation reversibility. Here, we report a bicontinuous, uniaxially aligned liquid crystal elastomer-hydrogel composite (BALCEH) that allows both multi-stimuli shape reconfiguration and solvent-driven self-propulsion. The material integrates hydrophilic and hydrophobic networks, resulting in asymmetric solvent uptake and directional swelling across both aqueous and non-aqueous environments. This architecture supports reversible actuation under humidity, temperature, and organic solvents, governed by the interplay between anisotropic hydrogel expansion and LCE elasticity. BALCEH also achieves sustained Marangoni propulsion, with trajectory programmability through fuel composition and geometry. Additionally, spatial rearrangement of the dual networks imparts adaptive wettability, switching between superoleophobic and superhydrophobic states. By coupling deformation and motion in a single system, BALCEH offers a versatile platform for untethered soft robotics and intelligent, reconfigurable materials.
Similar content being viewed by others
Data availability
The data that support the findings of this study are included within the Article and its Supplementary Information. Raw data can be obtained from the corresponding author upon request. Source data are provided with this paper as a source data file. Source data are provided with this paper.
References
Dawson, C., Vincent, J. F. V. & Rocca, A.-M. How pine cones open. Nature 390, 668–668 (1997).
Eger, C. J. et al. The structural and mechanical basis for passive-hydraulic pine cone actuation. Adv. Sci. 9, 2200458 (2022).
Guo, Q. et al. Fast nastic motion of plants and bioinspired structures. J. R. Soc. Interface 12, 20150598 (2015).
Ke, X., Yong, H., Xu, F., Ding, H. & Wu, Z. Stenus-inspired, swift, and agile untethered insect-scale soft propulsors. Nat. Commun. 15, 1491 (2024).
Dietz, A. A., Hofmann, M. J. & Motschmann, H. The role of surface viscosity in the escape mechanism of the Stenus beetle. J. Phys. Chem. B 120, 7143–7147 (2016).
Scriven, L. & Sterling, C. The Marangoni effects. Nature 187, 186–188 (1960).
Alexandre, P. et al. The mechanical world of bacteria. Cell 161, 988–997 (2015).
Herbert, K. M. et al. Synthesis and alignment of liquid crystalline elastomers. Nat. Rev. Mater. 7, 23–38 (2022).
Nie, Z. Z., Wang, M. & Yang, H. Structure-induced intelligence of liquid crystal elastomers. Chem. Eur. J. 29, e202301027 (2023).
Jiang, Z.-C., Liu, Q., Xiao, Y.-Y. & Zhao, Y. Liquid crystal elastomers for actuation: A perspective on structure-property-function relation. Prog. Polym. Sci. 153, 101829 (2024).
Lim, D. Hydrophilic gels for biological use. Nature 185, 4706 (1960).
Buwalda, S. J. et al. Hydrogels in a historical perspective: from simple networks to smart materials. J. Control. Release 190, 254–273 (2014).
Sano, K., Ishida, Y. & Aida, T. Synthesis of anisotropic hydrogels and their applications. Angew. Chem. Int. Ed. 57, 2532–2543 (2018).
Pinchin, N. P. et al. Liquid crystal networks meet water: it’s complicated!. Adv. Mater. 36, 2303740 (2024).
Stumpel, J. E. et al. Stimuli-responsive materials based on interpenetrating polymer liquid crystal hydrogels. Adv. Funct. Mater. 25, 3314–3320 (2015).
Deng, Z., Zhou, G. & de Haan, L. T. Preparation of an interpenetrating network of a poly (ampholyte) and a cholesteric polymer and investigation of its hydrochromic properties. ACS Appl. Mater. Interfaces 11, 36044–36051 (2019).
Shi, X. et al. Wearable optical sensing of strain and humidity: a patterned dual-responsive semi-interpenetrating network of a cholesteric main-chain polymer and a poly (ampholyte). Adv. Funct. Mater. 31, 2104641 (2021).
Zhang, L. et al. Preparation and properties of water-responsive films with color controllable based on liquid crystal and poly (ethylene glycol) interpenetrating polymer network. Liq. Cryst. 49, 1411–1419 (2022).
Kim, K. et al. 4D printing of hygroscopic liquid crystal elastomer actuators. Small 17, 2100910 (2021).
Xu, L., Zhang, S., Yin, L. & Zhao, Y. Humidity-sensing and moisture-steering liquid crystal elastomer actuator. Small 21, 2412547 (2025).
Harris, K. D., Bastiaansen, C. W. M., Lub, J. & Broer, D. J. Self-assembled polymer films for controlled agent-driven motion. Nano Lett. 5, 1857–1860 (2005).
De Haan, L. T., Verjans, J. M. N., Broer, D. J., Bastiaansen, C. W. M. & Schenning, A. P. H. J. Humidity-responsive liquid crystalline polymer actuators with an asymmetry in the molecular trigger that bend, fold, and curl. J. Am. Chem. Soc. 136, 10585–10588 (2014).
Wang, Z. et al. Reprogrammable humidity-driven liquid crystalline polymer actuator enabled by dynamic ionic bonds. ACS Appl. Mater. Interfaces 14, 17869–17877 (2022).
Lan, R. et al. Reversibly and irreversibly humidity-responsive motion of liquid crystalline network gated by SO2 gas. Adv. Funct. Mater. 29, 1900013 (2019).
Hu, W. et al. Humidity-responsive blue phase liquid-crystalline film with reconfigurable and tailored visual signals. Adv. Funct. Mater. 30, 2004610 (2020).
Liu, Y. et al. Humidity-and photo-induced mechanical actuation of cross-linked liquid crystal polymers. Adv. Mater. 29, 1604792 (2017).
Zheng, X. et al. A cut-and-weld process to 3D architectures from multiresponsive crosslinked liquid crystalline polymers. Small 15, 1900110 (2019).
Wani, O. M., Verpaalen, R., Zeng, H., Priimagi, A. & Schenning, A. P. H. J. An artificial nocturnal flower via humidity-gated photoactuation in liquid crystal networks. Adv. Mater. 31, 1805985 (2019).
Sun, H., Chai, X., Yang, H., Wei, J. & Yu, Y. Photo-and humidity-responsive liquid crystal copolymer actuators fabricated via vapor-assisted alignment. ACS Appl. Mater. Interfaces 16, 15405–15415 (2024).
Gladman, A. S., Matsumoto, E. A., Mahadevan, L. & Lewis, J. A. Biomimetic 4D printing. Nat. Mater. 15, 413–418 (2016).
Zhu, Q. L. et al. Light-steered locomotion of muscle-like hydrogel by self-coordinated shape change and friction modulation. Nat. Commun. 11, 5166 (2020).
Liu, M. et al. An anisotropic hydrogel with electrostatic repulsion between cofacially aligned nanosheets. Nature 517, 68–72 (2015).
Wu, L. et al. Magnetically induced anisotropic orientation of graphene oxide locked by in situ hydrogelation. ACS Nano 8, 4640–4649 (2014).
Zhu, Z. et al. Tough and thermosensitive poly (N-isopropylacrylamide)/graphene oxide hydrogels with macroscopically oriented liquid crystalline structures. ACS Appl. Mater. Interfaces 8, 15637–15644 (2016).
Qin, H., Zhang, T., Li, N., Cong, H.-P. & Yu, S.-H. Anisotropic and self-healing hydrogels with multi-responsive actuating capability. Nat. Commun. 10, 2202 (2019).
Yang, X. et al. Ordered gelation of chemically converted graphene for next-generation electroconductive hydrogel films. Angew. Chem. Int. Ed. 50, 7325–7328 (2011).
Choi, S., Choi, Y. & Kim, J. Anisotropic hybrid hydrogels with superior mechanical properties reminiscent of tendons or ligaments. Adv. Funct. Mater. 29, 1904342 (2019).
Lin, P., Zhang, T., Wang, X., Yu, B. & Zhou, F. Freezing molecular orientation under stretch for high mechanical strength but anisotropic hydrogels. Small 12, 4386–4392 (2016).
Ye, S., Ma, W. & Fu, G. Anisotropic hydrogels constructed via a novel bilayer-co-gradient structure strategy toward programmable shape deformation. Chem. Mater. 35, 999–1007 (2023).
Li, J. et al. Highly bidirectional bendable actuator engineered by LCST–UCST bilayer hydrogel with enhanced interface. ACS Appl. Mater. Interfaces 12, 55290–55298 (2020).
Wu, S. et al. Aggregation-induced emissive carbon dots gels for octopus-inspired shape/color synergistically adjustable actuators. Angew. Chem. Int. Ed. 60, 21890–21898 (2021).
Takahashi, R. et al. Control superstructure of rigid polyelectrolytes in oppositely charged hydrogels via programmed internal stress. Nat. Commun. 5, 4490 (2014).
Kim, D. S., Lee, Y.-J., Kim, Y. B., Wang, Y. & Yang, S. Autonomous, untethered gait-like synchronization of lobed loops made from liquid crystal elastomer fibers via spontaneous snap-through. Sci. Adv. 9, eadh5107 (2023).
Dhar, M., Das, A., Parbat, D. & Manna, U. Designing a network of crystalline polymers for a scalable, nonfluorinated, healable and amphiphobic solid slippery interface. Angew. Chem. 134, e202116763 (2022).
Sarma, H. et al. Highly water-rich robust coating for separating immiscible liquids mixtures of wide range of surface tension differences. Adv. Funct. Mater. 34, 2403607 (2024).
Liu, Z. et al. Multiple hydrogen-bonded cross-linked photo-responsive liquid crystal elastomers with photo-responsive fluorescence. Polymer 215, 123420 (2021).
Gao, H. et al. Adaptive and freeze-tolerant heteronetwork organohydrogels with enhanced mechanical stability over a wide temperature range. Nat. commun. 8, 15911 (2017).
Rather, A. M. et al. Color morphing surfaces with effective chemical shielding. Nat. Commun. 15, 3735 (2024).
Sun, L. et al. Bioinspired programmable wettability arrays for droplet manipulation. Proc. Natl. Acad. Sci. USA 117, 4527–4532 (2020).
Yao, Y. et al. Wettability-based ultrasensitive detection of amphiphiles through directed concentration at disordered regions in self-assembled monolayers. Proc. Natl. Acad. Sci. USA 119, e2211042119 (2022).
Ryu, M., Yoon, J., Chae, M., Chun, H. J. & Lee, H. Multi-level wettability patterned porous matrix for advanced optical information encryption. Adv. Funct. Mater. 35, 2414242 (2025).
Yu, B., Hu, H., Li, J., Ding, X. & Li, Z. Wetting-enabled microfluidic surface for fluid/droplet manipulation: fabrication, strategies, and applications. Adv. Eng. Mater. 26, 2400200 (2024).
Wang, Z., Boechler, N. & Cai, S. Anisotropic mechanical behavior of 3D printed liquid crystal elastomer. Addit. Manuf. 52, 102678 (2022).
Terentjev, E. M. Liquid crystal elastomers: 30 years after. Macromolecules 58, 2792–2806 (2025).
Speregen, J. M. & White, T. J. Liquid crystalline elastomers in soft robotics: assessing promise and limitations. Adv. Robot. Res. e202500150 (2025).
Barnes, M., Cetinkaya, S., Ajnsztajn, A. & Verduzco, R. Understanding the effect of liquid crystal content on the phase behaviour and mechanical properties of liquid crystal elastomers. Soft Matter 18, 5074–5081 (2022).
Cang, Y. et al. On the origin of elasticity and heat conduction anisotropy of liquid crystal elastomers at gigahertz frequencies. Nat. Commun. 13, 5248 (2022).
Merkel, D. R., Traugutt, N. A., Visvanathan, R., Yakacki, C. M. & Frick, C. P. Thermomechanical properties of monodomain nematic main-chain liquid crystal elastomers. Soft Matter 14, 6024–6036 (2018).
Okamoto, S., Sakurai, S. & Urayama, K. Effect of stretching angle on the stress plateau behavior of main-chain liquid crystal elastomers. Soft Matter 17, 3128–3136 (2021).
Yang, R. & Zhao, Y. Non-uniform optical inscription of actuation domains in a liquid crystal polymer of uniaxial orientation: an approach to complex and programmable shape changes. Angew. Chem. 129, 14390–14394 (2017).
Roach, D. J. et al. Long liquid crystal elastomer fibers with large reversible actuation strains for smart textiles and artificial muscles. ACS Appl. Mater. Interfaces 11, 19514–19521 (2019).
Xiao, M., Xian, Y. & Shi, F. Precise macroscopic supramolecular assembly by combining spontaneous locomotion driven by the Marangoni effect and molecular recognition. Angew. Chem. Int. Ed. 54, 9070–9074 (2015).
Yu, H. et al. Marangoni effect enabling autonomously miniatured swimmers: mechanisms, design strategy, and applications. Adv. Funct. Mater. 35, e202424235 (2025).
Bormashenko, E. et al. Superposition of translational and rotational motions under self-propulsion of liquid marbles filled with aqueous solutions of camphor. Langmuir 33, 13184–13189 (2017).
Bormashenko, E. et al. Self-propulsion of liquid marbles: Leidenfrost-like levitation driven by Marangoni flow. J. Phys. Chem. C. 119, 9910–9915 (2015).
Ooi, C. H. et al. A floating self-propelling liquid marble containing aqueous ethanol solutions. RSC Adv. 5, 101006–101012 (2015).
Barman, N. et al. Regulating the self-propulsion of liquid marbles on a water pool. Adv. Funct. Mater. 35, e05295 (2025).
Barnes, M. & Verduzco, R. Direct shape programming of liquid crystal elastomers. Soft Matter 15, 870–879 (2019).
Yakacki, C. M. et al. Tailorable and programmable liquid-crystalline elastomers using a two-stage thiol–acrylate reaction. RSC Adv. 5, 18997–19001 (2015).
Bauman, G. E., McCracken, J. M. & White, T. J. Actuation of liquid crystalline elastomers at or below ambient temperature. Angew. Chem. Int. Ed. 61, e202202577 (2022).
Zhao, Y. et al. Double cross-linked biomimetic hyaluronic acid-based hydrogels with thermo-stimulated self-contraction and tissue adhesiveness for accelerating post-wound closure and wound healing. Adv. Funct. Mater. 33, 2300710 (2023).
Mandal, S., Vignesh, A., Debnath, S. & Ojha, U. Mechanically robust anisotropic hydrogel–organogel conjugates for soft actuators with fast response time and diverse bi-axial programmable folding ability. Chem. Mater. 34, 5125–5137 (2022).
Mahajan, A., Singh, A., Datta, D. & Katti, D. S. Bioinspired injectable hydrogels dynamically stiffen and contract to promote mechanosensing-mediated chondrogenic commitment of stem cells. ACS Appl. Mater. Interfaces 14, 7531–7550 (2022).
Li, T. et al. Ultrastable piezoelectric biomaterial nanofibers and fabrics as an implantable and conformal electromechanical sensor patch. Sci. Adv. 10, eadn8706 (2024).
Acknowledgements
U.M. acknowledges generous financial support from Anusandhan National Research Foundation (CRG/2022/000710; SERB) and the Ministry of Electronics and Information Technology (no. 5(1)/2022-NANO). We acknowledge the generous support from Prof. E. Bhoje Gowd in performing WAXS. U.M. thanks the Department of Chemistry, Centre for Nanotechnology, Central Instrumental Facility, Indian Institute of Technology, Guwahati. P.G. thanks MoE and the institute for his doctoral fellowship.
Author information
Authors and Affiliations
Contributions
P.G. performed all the experiments with the help of A.B., D.S., S.D., A.H.W., H.S., and A.M. P.G. and A.B. designed experiments and analyzed data together. U.M. conceived the idea, U.M. and X.W. supervised the work together, U.M. wrote the manuscript, and all authors contributed to editing and reviewing the manuscript.
Corresponding authors
Ethics declarations
Competing interests
The authors declare no competing interests.
Peer review
Peer review information
Nature Communications thanks Wei Feng, Fuhua Xue, and the other, anonymous, reviewer for their contribution to the peer review of this work. A peer review file is available.
Additional information
Publisher’s note Springer Nature remains neutral with regard to jurisdictional claims in published maps and institutional affiliations.
Supplementary information
Source data
Rights and permissions
Open Access This article is licensed under a Creative Commons Attribution-NonCommercial-NoDerivatives 4.0 International License, which permits any non-commercial use, sharing, distribution and reproduction in any medium or format, as long as you give appropriate credit to the original author(s) and the source, provide a link to the Creative Commons licence, and indicate if you modified the licensed material. You do not have permission under this licence to share adapted material derived from this article or parts of it. The images or other third party material in this article are included in the article’s Creative Commons licence, unless indicated otherwise in a credit line to the material. If material is not included in the article’s Creative Commons licence and your intended use is not permitted by statutory regulation or exceeds the permitted use, you will need to obtain permission directly from the copyright holder. To view a copy of this licence, visit http://creativecommons.org/licenses/by-nc-nd/4.0/.
About this article
Cite this article
Giri, P., Borbora, A., Sarkar, D. et al. Coupling programmable shape morphing and solvent-fueled propulsion in a soft bicontinuous composite. Nat Commun (2026). https://doi.org/10.1038/s41467-026-69432-x
Received:
Accepted:
Published:
DOI: https://doi.org/10.1038/s41467-026-69432-x
