

FOLLOWUS
a.State Key Laboratory of Advanced Marine Materials, Ningbo Institute of Materials Technology and Engineering, Chinese Academy of Sciences, Ningbo 315201, China
b.School of Chemical Sciences, University of Chinese Academy of Sciences, Beijing 100049, China
tao.chen@nimte.ac.cn (T.C.)
luwei@nimte.ac.cn (W.L.)
Received:30 December 2025,
Accepted:27 January 2026,
Online First:17 April 2026,
Published:2026-03
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Yu, Y.; Zhou, W.; Chen, T.; Lu, W. Water swelling-induced stiffness enhancement of polymer hydrogels. Chinese J. Polym. Sci. https://doi.org/10.1007/s10118-026-3597-6
Yi Yu, Wei Zhou, Tao Chen, et al. Water Swelling-induced Stiffness Enhancement of Polymer Hydrogels[J/OL]. Chinese Journal of Polymer Science, 2026, 441-11.
Yu, Y.; Zhou, W.; Chen, T.; Lu, W. Water swelling-induced stiffness enhancement of polymer hydrogels. Chinese J. Polym. Sci. https://doi.org/10.1007/s10118-026-3597-6 DOI:
Yi Yu, Wei Zhou, Tao Chen, et al. Water Swelling-induced Stiffness Enhancement of Polymer Hydrogels[J/OL]. Chinese Journal of Polymer Science, 2026, 441-11. DOI: 10.1007/s10118-026-3597-6.
Polymer hydrogels with variable stiffness demonstrate immense practical application value
particularly when utilizing water as a trigger medium
which significantly expands their prospects in soft robotics
bioelectronics
and artificial muscles. However
existing water-induced stiffening hydrogel rely on ionic liquids and inorganic salts
posing leakage risks during prolonged use. Here
we proposed a strategy for mechanically strengthening hydrogel through water-induced phase separation. By designing a polymer matrix featuring hydrophilic oligomeric ethylene glycol methacrylate (OEGMA) and hydrophobic methyl methacrylate (MMA) moieties
this poly[methyl methacrylate-
co
-poly(ethylene glycol) methacrylate
]
[P(MMA
x
-
co
-OEGMA
y
)
]
hydrogel exhibited reversible stiffness switching across four orders of magnitude (from 1.88×10
–2
MPa to 201.63 MPa) upon water stimulation. This abrupt stiffness en
hancement stemmed from strong hydrogen bonding between water molecules and hydrophilic OEGMA segments
facilitating spontaneous aggregation and phase separation of hydrophobic MMA segments. The resulting hydrophobic MMA domains formed dynamic physical crosslinking points
thereby enhancing the hydrogel's stiffness. Furthermore
the hydrogel exhibited a time-dependent
multi-stage stiffness enhancement during water swelling. As proof of concept
it was employed as a shape-memory component to explore its application in the controllable programming of multi-stage complex shapes
offering novel design insights for developing environmentally friendly
high-mechanical-performance smart hydrogel materials.
Ganewatta, M. S.; Wang, Z.; Tang, C. Chemical syntheses of bioinspired and biomimetic polymers toward biobased materials. Nat. Rev. Chem. 2021 , 5 , 753−772..
Shanmuganathan, K.; Capadona, J. R.; Rowan, S. J.; Weder, C. Biomimetic mechanically adaptive nanocomposites. Prog. Polym. Sci. 2010 , 35 , 212−222..
Thurmond, F. A.; Trotter, J. A. Morphology and biomechanics of the microfibrillar network of sea cucumber dermis. J. Exp. Biol. 1996 , 199 , 1817−1828..
Szulgit, G. K.; Shadwick, R. E. Dynamic mechanical characterization of a mutable collagenous tissue: response of sea cucumber dermis to cell lysis and dermal extracts. J. Exp. Biol. 2000 , 203 , 1539−1550..
Mo, J.; Prévost, S. F.; Blowes, L. M.; Egertová, M.; Terrill, N. J.; Wang, W.; Elphick, M. R.; Gupta, H. S. Interfibrillar stiffening of echinoderm mutable collagenous tissue demonstrated at the nanoscale. Proc. Natl. Acad. Sci. 2016 , 113 , E 6362−E6371..
Hodick, D.; Sievers, A. On the mechanism of trap closure of venus flytrap (dionaea muscipula ellis). Planta 1989 , 179 , 32−42..
Forterre, Y.; Skotheim, J. M.; Dumais, J.; Mahadevan, L. How the venus flytrap snaps. Nature 2005 , 433 , 421−425..
Volkov, A. G.; Adesina, T.; Markin, V. S.; Jovanov, E. Kinetics and mechanism of dionaea muscipula trap closing. Plant Physiology 2008 , 146 , 323−324..
Duan, J.; Zhang, L. Robust and smart hydrogels based on natural polymers. Chinese J. Polym. Sci. 2017 , 35 , 1165−1180..
Wu, J. J.; Huang, L. M.; Zhao, Q.; Xie, T. 4D printing: history and recent progress. Chinese J. Polym. Sci . 2018 , 36 , 563−575..
Bao, B.; Zeng, Q.; Li, K.; Wen, J.; Zhang, Y.; Zheng, Y.; Zhou, R.; Shi, C.; Chen, T.; Xiao, C.; Chen, B.; Wang, T.; Yu, K.; Sun, Y.; Lin, Q.; He, Y.; Tu, S.; Zhu, L. Rap id fabrication of physically robust hydrogels. Nat. Mater. 2023 , 22 , 1253−1260..
Ishikawa, S.; Iwanaga, Y.; Uneyama, T.; Li, X.; Hojo, H.; Fujinaga, I.; Katashima, T.; Saito, T.; Okada, Y.; Chung, U.; Sakumichi, N.; Sakai, T. Percolation-induced gel-gel phase separation in a dilute polymer network. Nat. Mater. 2023 , 22 , 1564−1570..
Lin, X.; Wang, X.; Cui, H.; Rao, P.; Meng, Y.; Ouyang, G.; Guo, H. Hydrogels with ultra-highly additive adjustable toughness under quasi-isochoric conditions. Mater. Horiz. 2023 , 10 , 993−1004..
[Liu, C.; He, C.; Dai, X.; Yan, L.; Xu, H. Achieving mechanical evolution in polymer materials through phase evolution induced by visible light. Adv. Mater . 2025 , e08549..
Chen, L.; Yin, Y.; Liu, Y.; Lin, L.; Liu, M. Design and fabrication of functional hydrogels through interfacial engineering. Chinese J. Polym. Sci. 2017 , 35 , 1181−1193..
Zhang, Y.; Zhao, W.; Ma, S.; Liu, H.; Wang, X.; Zhao, X.; Yu, B.; Cai, M.; Zhou, F. Modulus adaptive lubricating prototype inspired by instant muscle hardening mechanism of catfish skin. Nat. Commun. 2022 , 13 , 377..
Wu, J.; Wu, B.; Xiong, J.; Sun, S.; Wu, P. Entropy-mediated polymer-cluster interactions enable dramatic thermal stiffening hydrogels for mechanoadaptive smart fabrics. Angew. Chem. Int. Ed. 2022 , 61 , e202204960..
Liu, D.; Jiang, P.; Wang, Y.; Lu, Y.; Wu, J.; Xu, X.; Ji, Z.; Sun, C.; Wang, X.; Liu, W. Engineering tridimensional hydrogel tissue and organ phantoms with tunable springiness. Adv. Funct. Mater. 2023 , 33 , 2214885..
Han, Y. Q.; Lei, Z. Y.; Wu, P.Y. Mxene nanosheet-enhanced ionotronic hydrogels for wireless powering and noncontact sensing. Chinese J. Polym. Sci. 2025 , 43 , 572−580..
Chen, D.; Wang, H. J.; Ni, C. J.; Chen, J. Y.; Guo, Y. J.; Chen, Z.; Zheng, N.; Wu, J. J.; Ren, H.; Zhao, Q. Light-regulated microstructure growth of dynamic hydrogels for flexible manufacturing of microlens arrays. Chem Bio Eng. 2025 , 2 , 350−357..
Li, J. S.; Hu, Z. Q.; Zhang, H. W.; Ji, X. F. Poly[2 ] catenanes-based hydrogels prepared by hydroxyl-yne click chemistry. Supramolecular Materials 2024 , 3 , 100076..
Qiu, J. X.; Ma, H. D.; Yao, M. T.; Song, M. T.; Zhang, L. P.; Xu, J. K.; Liu, X. M.; Lu, B. Y. Design of a supersoft, ultra-stretchable, and 3d printable hydrogel electrical bioadhesive interface for electromyography monitoring. Supramolecular Materials 2024 , 3 , 100079..
Lu, W.; Si, M. Q.; Le, X. X.; Chen, T. Mimicking color-changing organisms to enable the multicolors and multifunctions of smart fluorescent polymeric hydrogels. Acc. Chem. Res. 2022 , 55 , 2291−2303..
Feng, W. H.; Li, F.; Jiang, Z. Y.; Yue, C. J.; Yin, G. Q.; Zhu, N.; Zhang, K.; Chen, T.; Lu, W. Supramolecular entanglement driven emissive aggregate densification enabling room-temperature phosphorescence hydrogels with ultrastretchability and crack-tolerance. Angew. Chem. Int. Ed. 2025 , 64 , e202505192..
Zhou, Y.; Yu, C.; Zhang, X.; Zheng, Y.; Wang, B.; Bao, Y.; Shan, G.; Wang, H.; Pan, P. Ultrasensitive ionic conductors with tunable resistance switching temperature enabled by phase transformation of polymer cocrystals. Adv. Mater. 2024 , 36 , 2309568..
Zhao, X.; Peng, L. M.; Chen, Y.; Zha, X. J.; Li, W. D.; Bai, L.; Ke, K.; Bao, R. Y.; Yang, M. B.; Yang, W. Phase change mediated mechanically transformative dynamic gel for intelligent control of versatile devices. Mater. Horiz. 2021 , 8 , 1230−1241..
Zhou, W.; Han, Y.; Xiao, P.; Yu, Y.; Wang, Y. C.; Chen, T. Interfacial elastic film with temperature mediated-phase transition behavior for tunable suspended sensing. Chinese J. Polym. Sci. 2025 , 43 , 1155−1162..
Nonoyama, T.; Lee, Y. W.; Ota, K.; Fujioka, K.; Hong, W.; Gong, J. P. Instant thermal switching from soft hydrogel to rigid plastics inspired by thermophile proteins. Adv. Mater. 2020 , 32 , 1905878..
Zhao, Y.; Wu, B.; Sun, S.; Wu, P. Chemical fuel-driven stiffening of transient hydrogels via vitrifiable phase separation. Angew. Chem. Int. Ed. 2025 , 64 , e202518064..
Li, H. B.; Bian, Q. Y. Stimuli-responsive protein hydrogels: from dynamic tuning of hydrogel mechanics to shape morphing. Supramolecular Materials. 2025 , 4 , 100120..
[Wei, M.; Han, J. Y.; Yu, C.; Li, P.; Zhang, X. Y.; Ding, J. H.; Chen, M. W.; Li, X. K.; Yin, G. Q.; Zhang, T.; Wang, J. G.; Théato, P; Chen, T.; Lu, Wei. Mass diffusion-dominated phase separation enabling on-demand and repeatable lifetime programming of room-temperature phosphorescence polymer hydrogels. Adv. Mater . 2025 , e17109..
Ming, X.; Zhang, D.; Zhu, H.; Zhang, Q.; Zhu, S. Tremendous stiffness-changing polymer networks enabled by touch-induced crystallization. Adv. Funct. Mater. 2024 , 34 , 2411560..
Wang, S.; Liu, H.; Yu, Z.; Ren, X.; Hua, Q.; Panahi-Sarmad, M.; Yang, P.; Liu, C.; Renneckar, S.; Liu, H.; Jiang, F. Cellulose-mediated ionic liquid crystallization enables tough-stiff switchable ionogels. Nat. Commun. 2025 , 16 , 9007..
Lee, J.; Castilho, R. M.; Nam, S. Spatiotemporal toughness modulation in hydrogels through on-demand cross-linking. Sci. Adv. 2025 , 11 , eadz0440..
Hou, R.; Xu, L. J.; Yu, M. L.; Tang, Z. M.; Zhou, B.; Zhang, Q.; Li, N.; Xu, J. X. Piezoelectric-triboelectric hybrid nanogenerator based on tough, stretchable batio 3 doped antibacterial hydrogel for self-powered sensors. Supramolecular Materials 2025 , 4 , 100096..
Yan, D. D.; Zhu, S. L.; Zhao, H. Y.; Feng, S. H; Kang, B. B.; Yang, X.; Zhang, Y. J.; Li, Z. Z.; Yu, W. W.; Ye, Y. N. Organic-inorganic nanocomposite organogel with double-network topologyfor enhanced mechanical and dielectric properties. Supramolecular Materials 2025 , 4 , 100112..
[Wu, Z.; Kong, H.; Wang, J.; Guan, J.; Yin, M. Photo-responsive peptide hydrogels with tunable stiffness via water switching for cell fate regulation. Adv. Funct. Mater . 2025 , e26641..
Ma, M.; Guo, L.; Anderson, D. G.; Langer, R. Bio-inspired polymer composite actuator and generator driven by water gradients. Science 2013 , 339 , 186−189..
Itagaki, H.; Kurokawa, T.; Furukawa, H.; Nakajima, T.; Katsumoto, Y.; Gong, J. P. Water-induced brittle-ductile transition of double network hydrogels. Macromolecules 2010 , 43 , 9495−9500..
Gong, K.; Hou, L.; Wu, P. Hydrogen-bonding affords sustainable plastics with ultrahigh robustness and water-assisted arbitrarily shape engineering. Adv. Mater. 2022 , 34 , 2201065..
[Xu, Z.; Wu, M.; Gao, W.; Bai, H. A sustainable single-component “silk nacre.” Sci. Adv . 2022 , 8 , eabo0946..
Yang, C.; Zheng, W. Z.; Ni, C.J.; Li, Y.;Chen, D.; Xie, T.; Zhao, Q. Reconfigurable and orthogonal stiffness-structure patterning of dynamically crosslinked amphigels. SmartMat. 2024 , 5 , e1255..
Wang, Z.; Qiu, W.; Zhang, Q. Constructing phase separation in polymer gels: strategies, functions and applications. Prog. Polym. Sci. 2024 , 154 , 101847..
Xu, J.; Bohnsack, D. A.; Mackay, M. E.; Wooley, K. L. Unusual mechanical performance of amphiphilic crosslinked polymer networks. J. Am. Chem. Soc. 2007 , 129 , 506−507..
Bedoui, F.; Widjaj a, L. K.; Luk, A.; Bolikal, D.; Murthy, N. S.; Kohn, J. Anomalous increase in modulus upon hydration in random copolymers with hydrophobic segments and hydrophilic blocks. Soft Matter 2012 , 8 , 2230..
Ming, X.; Yao, L.; Zhu, H.; Zhang, Q.; Zhu, S. Dramatic and reversible water-induced stiffening driven by phase separation within polymer gels. Adv. Funct. Mater. 2022 , 32 , 2109850..
Xu, J.; Wu, B.; Hou, L.; Wu, P. Hydrogen bonding competition mediated phase separation with abnormal moisture-induced stiffness boosting. Small 2024 , 20 , 2401164..
Li, M.; Lu, H.; Pi, M.; Zhou, H.; Wang, Y.; Yan, B.; Cui, W.; Ran, R. Water-induced phase separation for anti-swelling hydrogel adhesives in underwater soft electronics. Adv. Sci. 2023 , 10 , 2304780..
Yu, K.; Feng, Z.; Du, H.; Lee, K. H.; Li, K.; Zhang, Y.; Masri, S. F.; Wang, Q. Constructive adaptation of 3d-printable polymers in response to typically destructive aquatic environments. PNAS Nexus 2022 , 1 , pgac139..
Shibayama, M. Smal l-angle neutron scattering on polymer gels: phase behavior, inhomogeneities and deformation mechanisms. Polym. J. 2011 , 43 , 18−34..
Ikemoto, Y.; Harada, Y.; Tanaka, M.; Nishimura, S.; Murakami, D.; Kurahashi, N.; Moriwaki, T.; Yamazoe, K.; Washizu, H.; Ishii, Y.; Torii, H. Infrared spectra and hydrogen-bond configurations of water molecules at the interface of water-insoluble polymers under humidified conditions. J. Phys. Chem. B 2022 , 126 , 4143−4151..
Yao, X.; Dunn, S. S.; Kim, P.; Duffy, M.; Alvarenga, J.; Aizenberg, J. Fluorogel elastomers with tunable transparency, elasticity, shape-memory, and antifouling properties. Angew. Chem. Int. Ed. 2014 , 53 , 4418−4422..
Ren, Y.; Liu, Z.; Jin, G.; Yang, M.; Shao, Y.; Li, W.; Wu, Y.; Liu, L.; Yan, F. Electric-field-induced gradient ionogels for highly sensitive, broad-range-response, and freeze/heat-resistant ionic fingers. Adv. Mater. 2021 , 33 , 2008486..
Li, M.; Chen, L.; Li, Y.; Dai, X.; Jin, Z.; Zhang, Y.; Feng, W.; Yan, L.-T.; Cao, Y.; Wang, C. Superstretchable, yet stiff, fatigue-resistant ligament-like elastomers. Nat. Commun. 2022 , 13 , 2279..
Sel, E.; Ulu, A.; Ateş, B.; Köytepe, S. Comparative study of catalase immobilization via adsorption on p(mma-co-peg500ma) structures as an effective polymer support. Polym. Bull. 2021 , 78 , 2663−2684..
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