Strong and Tough High-water Content Double-network Hydrogels

Shu-Xing Yin; Guo-Jun Che; Cheng Qian; Meng Yu; Can Zhou; Sheng-Wen Kong; Chuang-Qi Zhao; Lei Jiang

doi:10.1007/s10118-026-3684-8

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Strong and Tough High-water Content Double-network Hydrogels

Special Topic: Functional Gels | Updated：2026-05-30

- Strong and Tough High-water Content Double-network Hydrogels
- Strong and Tough High-water Content Double-network Hydrogels
- Chinese Journal of Polymer Science 2026年44卷第6期页码：1738-1748
- Affiliations：
  
  a.State Key Laboratory of Bioinspired Interfacial Materials Science, School of Chemistry and Materials Science, University of Science and Technology of China, Hefei 230026, China
  b.State Key Laboratory of Bioinspired Interfacial Materials Science, Suzhou Institute for Advanced Research, University of Science and Technology of China, Suzhou 215123, China
- Author bio：
  
  kongsw@ustc.edu.cn (S.W.K.)
  zhaochuangqi@ustc.edu.cn (C.Q.Z.)
- Funds：
  
  This work was financially supported by the National Natural Science Foundation of China (Nos. 22305244 and 2252200918), CAS Hundred Talent Program (No. KJ2060007007), and Suzhou Key Laboratory of Bioinspired Interfacial Science (No. SZ2024004). This research was also supported by the Physical and Chemical Analysis Center of the Suzhou Institute for Advanced Research, University of Science and Technology of China.;The authors declare no interest conflict.Electronic supplementary information (ESI) is available free of charge in the online version of this article at http://doi.org/10.1007/s10118-026-3684-8.The data supporting the findings of this study are available from the corresponding author upon reasonable request. Author’s contact information: kongsw@ustc.edu.cn and zhaochuangqi@ustc.edu.cn.
- DOI：10.1007/s10118-026-3684-8
  中图分类号：
- 收稿：2026-02-27，
  
  录用：2026-03-26，
  
  网络首发：2026-05-20，
  
  纸质出版：2026-06-05
- Accepted：
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Yin, S. X.; Che, G. J.; Qian, C.; Yu, M.; Zhou, C.; Kong, S. W.; Zhao, C. Q.; Jiang, L. Strong and tough high-water content double-network hydrogels. Chinese J. Polym. Sci. 2026, 44, 1738–1748

Shu-Xing Yin, Guo-Jun Che, Cheng Qian, et al. Strong and Tough High-water Content Double-network Hydrogels[J]. Chinese Journal of Polymer Science, 2026, 44(6): 1738-1748.
Yin, S. X.; Che, G. J.; Qian, C.; Yu, M.; Zhou, C.; Kong, S. W.; Zhao, C. Q.; Jiang, L. Strong and tough high-water content double-network hydrogels. Chinese J. Polym. Sci. 2026, 44, 1738–1748 DOI： 10.1007/s10118-026-3684-8.

Shu-Xing Yin, Guo-Jun Che, Cheng Qian, et al. Strong and Tough High-water Content Double-network Hydrogels[J]. Chinese Journal of Polymer Science, 2026, 44(6): 1738-1748. DOI： 10.1007/s10118-026-3684-8.

摘要

This study proposes a strategy to fabricate strong and tough double-network hydrogels through multiple freeze-thaw cycles. Network densification endows hydrogels with exceptional mechanical performance. Moreover

the hydrogel possessed a high water content (up to 95%) and excellent biocompatibility.

Abstract

Hydrogels have been widely used in tissue engineering and biomedical applications owing to their high water content and tunable functionality. Nevertheless

high water content and loosely cross-linked networks restrict the mechanical properties of hydrogels and their practical applications. Herein

we present a facile approach for designing strong and tough bacterial cellulose/poly(vinyl alcohol) (BC/PVA) double-network hydrogels involving immersing BC into PVA solutions and then freezing-thawing. The PVA chains encapsulate the BC nanofibers through hydrogen bonding interactions and chain entanglement

infiltrate the fibrous network

and thereby enhance the densification of the BC/PVA hydrogel. Concurrently

repetitive freeze-thaw cycles facilitate the regulation of PVA chain conformation and promote PVA crystallization

which increases the rigidity of the PVA segments. The resulted hydrogel demonstrates an exceptional tensile strength of (2.13±0.03) MPa

a remarkable toughness of (1.15±0.03) MJ·m

–3

and a high water content of up to 95%. Furthermore

the double-network hydrogels exhibit excellent biocompatibility. This study offers a practical strategy for the design of robust and tough hydrogels with potential utility in biomedical applications.

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Keywords

references

Zhao, X.; Chen, X.; Yuk, H.; Lin, S.; Liu, X.; Parada, G. Soft materials by design: unconventional polymer networks give extreme properties. Chem. Rev. 2021 , 121 , 4309−4372..

Zhang, Q.; Liu, Y.; Yang, G.; Kong, H.; Guo, L.; Wei, G. Recent advances in protein hydrogels: from design, structural and functional regulations to healthcare applications. Chem. Eng. J. 2023 , 451 , 138494..

[Zhang, L.; Lee, W.; Li, X.; Jiang, Y.; Fang, X.; Dai, G.; Liu, Y. 3D direct printing of mechanical and biocompatible hydrogel meta-structures. Bioact. Mater . 2022 , 10 , 48−55..

Liu, Z.; Zhang, H.; Zhou, R.; Gao, H.; Wu, Y.; Wang, Y.; Wu, H.; Guan, C.; Wang, L.; Tang, L.; Song, P.; Xue, H.; Gao, J. Thermoplastic elastomer-reinforced hydrogels with excellent mechanical properties, swelling resistance, and biocompatibility. Adv. Sci. 2025 , 12 , 2414339..

Xiao, W.; Wu, H.; Su, Q.; Yan, J.; Tang, L.; Huang, X.; Lu, L.; Gu, W.; Song, P.; Gao, J. MXene initiated in situ construction of superhydrophobic and electrically conductive nanofibrous composites for wearable multifunctional sensing. Chem. Eng. J. 2025 , 508 , 161074..

Peng, R.; Ba, F.; Li, J.; Cao, J.; Zhang, R.; Liu, W.-Q.; Ren, J.; Liu, Y.; Li, J.; Ling, S. Embedding living cells with a mechanically reinforced an d functionally programmable hydrogel fiber platform. Adv. Mater. 2023 , 35 , 2305583..

Zhou, D.; Wang, W.; Ma, W.; Xian, Y.; Zhang, Z.; Pan, Z.; Li, Y.; Huang, L.; Liu, L.; Zheng, Z.; Liu, H.; Wu, D. Cartilage-adaptive hydrogels via the synergy strategy of protein templating and mechanical training. Adv. Mater. 2025 , 37 , 2414081..

Asim, S.; Tuftee, C.; Qureshi, A. T.; Callaghan, R.; Geary, M. L.; Santra, M.; Pal, V.; Namli, I.; Yam, G.; Ozbolat, I. T.; Rizwan, M. Multi-functional gelatin-dithiolane hydrogels for tissue engineering. Adv. Funct. Mater. 2025 , 35 , 2407522..

López-Díaz, A.; Vázquez, A. S.; Vázquez, E. Hydrogels in soft robotics: past, present, and future. ACS Nano 2024 , 18 , 20817−20826..

Nasseri, R.; Bouzari, N.; Huang, J.; Golzar, H.; Jankhani, S.; Tang, X.; Mekonnen, T.-H.; Aghakhani, A.; Shahsavan, H. Programmable nanocomposites of cellulose nanocrystals and zwitterionic hydrogels for soft robotics. Nat. Commun. 2023 , 14 , 6108..

Fu, D.; Xing, L.; Xie, Y.; Li, P.; Yang, F.; Sui, X.; Liu, J.; Chi, J.; Huang, B.; Shen, J. Hybrid crosslinking cellulose nanofibers-reinforced zwitterionic poly (ionic liquid) organohydrogel with high-stretchable, anti-freezing, anti-drying as strain sensor application. Carbohyd. Polym. 2025 , 353 , 123253..

Gong, X.; Luo, Y.; Zhang, C.; Xie, J.; Wang, Y. Carboxymethyl chitosan-based tough hydrogels with low mechanical hysteresis and high conductivity as multifunctional sensors. Chem. Eng. J. 2025 , 510 , 161610..

Han, F.; Chen, S.; Wang, F.; Liu, M.; Li, J.; Liu, H.; Yang, Y.; Zhang, H.; Liu, D.; He, R.; Cao, W.; Qin, X.; Xu, F. High-conductivity, self-healing, and adhesive ionic hydrogels for health monitoring and human-machine interactions under extreme cold conditions. Adv. Sci. 2025 , 12 , 2412726..

Liu, H.; Guan, S.; Wang, P.; Dong, X. Super tough anti-freezing and antibacterial hydrogel with multi-crosslinked network for flexible strain sensor. Small 2025 , 21 , 2407870..

Liu, S.; Zhan, H.; Wu, P.; Lei, Z. Underwater-stable conductive hydrogels: From molecular design to next-generation aquatic sensors. Chin. J. Chem. 2026 , 44 , 571−582..

Xia, P.; Zhang, W.; Peng, C.; Yin, H.; Wang, D.; Yang, J.; Tuan, R.-S.; Jiang, L.; Wang, J. A high-order double network hydrogel. Macromolecules 2024 , 57 , 11251−11265..

[Fang, Y.; Liang, C.; Liljestrom, V.; Lv, Z.; Ikkala, O.; Zhang, H. Toughening hydrogels with fibrillar connected double networks. Adv. Mater . 2024 , 2402282..

Surhadi, J. U.; Aymon, B.; Carton, M.; Porerla, C. M. Double-network-inspired mechanical metamaterials. Nat. Mater. 2025 , 24 , 945−954..

Gu, Y.; Wu, W.; Zhang, C.; Li, X.; Guo, X.; Wang, Y.; Yuan, Y.; Jiang, B.; Jin, Y. Multi-solvent-induced gradient aggregation rendered superstrong, tough, stretchable, and fatigue-resistant lignin-based supramolecular hydrogels. Adv. Funct. Mater. 2025 , 35 , 2417206..

Hong, S.; Lee, J.; Park, T.; Jeong, J.; Lee, J.; Joo, H.; Mesa, J.; Alston, C.-B.; Ji, Y.; Vega, S. R.; Barinaga, C.; Yi, J.; Lee, Y.; Kim, J.; Won, K.; Solorio, L.; Kim, Y.; Lee, H.;Kim, D. R.; Lee, C. H. Spider silk-inspired conductive hydrogels for enhanced toughness and envir onmental resilience via dense hierarchical structuring. Adv. Sci. 2025 , 12 , 2500397..

Wu, S.; Liu, Z.; Gong, C.; Li, W.; Xu, S.; Wen, R.; Feng, W.; Qiu, Z.; Yan, Y. Spider-silk-inspired strong and tough hydrogel fibers with anti-freezing and water retention properties. Nat. Commun. 2024 , 15 , 4441..

Jiang, Y.; Tang, N.; Wang, X.; Pei, D.; Zhang, H.; Li, M.; Hu, J. Mechanically robust eutectogels enabled by precisely engineered crystalline domains. Nat. Commun. 2025 , 16 , 7417..

Tang, N.; Jiang, Y.; Wei, K.; Zheng, Z.; Zhang, H.; Hu, J. Evolutionary reinforcement of polymer networks: a stepwise-enhanced strategy for ultra-robust eutectogels. Adv. Mater. 2023 , 36 , 2309576..

Zhu, S.; Wang, S.; Huang, Y.; Tang, Q.; Fu, T.; Su, R.; Fan, C.; Xia, S.; Lee, P.-S.; Lin, Y. Bioinspired structural hydrogels with highly ordered hierarchical orientations by flow-induced alignment of nanofibrils. Nat. Commun. 2024 , 5 , 118..

Xu, L.; Qiao, Y.; Qiu, D. Coordinatively stiff en and toughen hydrogels with adaptable crystal-domain cross-linking. Adv. Mater. 2023 , 35 , 2209913..

Wu, Y.; Zhang, Y.; Wu, H.; Wen, J.; Zhang, S.; Xing, W.; Zhang, H.; Xue, H.; Gao, J.; Mai, Y. Solvent-exchange-assisted wet annealing: a new strategy for superstrong, tough, stretchable, and anti-fatigue hydrogels. Adv. Mater. 2023 , 35 , 2210624..

[Zhang, Y.; Liu, L.; Yin, S.; Zhou, C.; Ding, Y.; Che, G.; Zhao, C. Underwater high strength and tough polyvinyl alcohol-polyacrylic acid hydrogel. Adv. Funct. Mater . 2025 , 2503023..

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. Rapid fabrication of physically robust hydrogels. Nat. Mater. 2023 , 22 , 1253..

[Wang, S.; Yu, Z.; Sun, X.; Panahi-Sarmad, M.; Yang, P.; Zhu, P.; Zhu, Y.; Liu, H.; Jiang, F. A universal strategy to mitigate microphase separation via cellulose nanocrystal hydration in fabricating strong, tough, and fatigue-resistant hydrogels. Adv. Mater . 2024 , 2416916..

Kim, J.; Zhang, G.; Shi, M.; Suo, Z. Fracture, fatigue, and friction of polymers in which entanglements greatly outnumber cross-links. Science 2021 , 374 , 212−216..

Zhu, R.; Zhu, D.; Zheng, Z.; Wang, X. Tough double network hydrogels with rapid self-reinforcement and low hysteresis based on highly entangled networks. Nat. Commun. 2024 , 15 , 1344..

Liang, C.; Dudko, V.; Khoruzhenko, O.; Hong, X.; Lv, Z.; Tunn, I.; Umer, M.; Timonen, J.; Linder, M.-B.; Breu, J.; Ikkala, O.; Zhang, H. Stiff and self-healing hydrogels by polymer entanglements in co-planar nanoconfinement. Nat. Mater. 2025 , 24 , 599−606..

[Zhang, H.; Chen, L.; Xiao, Y.; Guo, X.; Zhao, S.; Guan, R.; Long, T.; Cheng, X.; Zhou, C. Development of strong and tough silicone hydrogels enabled by polymerization-induced microphase separation and multiscaled electrostatic interactions and their application as water-shrinkable sleeves. Adv. Funct. Mater . 2025 , e07061..

Huo, H.; Shen, J.; Wan, J.; Shi, H.; Yang, H.; Duan, X.; Gao, Y.; Chen, Y.; Kuang, F .; Li, H.; Yang, L.; Du, G. A tough and robust hydrogel constructed through carbon dots induced crystallization domains integrated orientation regulation. Nat. Commun. 2025 , 16 , 6221..

Fu, L.; Li, L.; Bian, Q.; Xue, B.; Jin, J.; Li, J.; Cao, Y.; Jiang, Q.; Li, H. Cartilage-like protein hydrogels engineered via entanglement. Nature 2023 , 618 , 740..

Picheth, G. F.; Pirich, C. L.; Sierakowski, M. R.; Woehl, M. A.; Sakakibara, C. N.; de Souza, C. F.; Martin, A.-A.; da Silva, R.; de Freitas, R. A. Bacterial cellulose in biomedical applications: A review. Int. J. Biol. Macromol. 2017 , 104 , 97−106..

Li, X.; Yuan, L.; Liu, R.; He, H.; Hao, J.; Lu, Y.; Wang, Y.; Liang, G.; Yuan, G.; Guo, Z. Engineering textile electrode and bacterial cellulose nanofiber reinforced hydrogel electrolyte to enable high-performance flexible all-solid-state supercapacitors. Adv. Energy Mater. 2021 , 11 , 2003010..

Nakayama, A.; Kakugo, A.; Gong, J.-P.; Osada, Y.; Takai, M.; Erata, T.; Kawano, S. High mechanical strength double-network hydrogel with bacterial cellulose. Adv. Funct. Mater. 2004 , 14 , 1124−1128..

Guan, Q.; Han, Z.; Zhu, Y.; Xu, W.; Yang, H.; Ling, Z.; Yan, B.; Yang, K.; Yin, C.; Wu, H.; Wu, H. Bio-inspired lotus-fiber-like spiral hydrogel bacterial cellulose fibers. Nano Lett. 2021 , 21 , 952−958..

Park, D.; Kim, J. W.; Shin, K.; Kim, J.-W. Bacterial cellulose nanofibrils-reinforced composite hydrogels for mechanical compression-responsive on-demand drug release. Carbohyd. Polym. 2021 , 272 , 118459..

Kim, J.; Choi, J.; Hyun, J. Free-form three-dimensional nanocellulose structure reinforced with poly(vinyl alcohol) using freeze-thaw process. Carbohyd. Polym. 2022 , 298 , 120055..

Liu, D.; Sun, X.; Tian, H.; Maiti, S.; Ma, Z. Effects of cellulose nanofibrils on the structure and properties on PVA nanocomposites. Cellulose 2013 , 20 , 2981−2989..

Soto-Bustamante, F.; Bassu, G.; Fratini, E.; Laurati, M. Effect of composition and freeze-thaw on the network structure, porosity and mechanical properties of polyvinyl-alcohol/chitosan hydrogels. Gels 2023 , 9 , 396..

[Wan, W.; Bannerman, A. D.; Yang, L.; Mak, H., in Polymeric cryogels , Springer, Switzerland, 2014 , p. 283..

Zhu, T.; Ni, Y.; Biesold, G. M.; Cheng, Y.; Ge, M.; Li, H.; Huang, J.; Lin, Z.; Lai, Y. Recent advances in conductive hydrogels: classifications, properties, and applications. Chem. Soc. Rev. 2023 , 52 , 473−509..

Eivazzadeh-Keihan, R.; Noruzi, E. B.; Aliabadi, H. A. M.; Sheikhaleslami, S.; Akbarzadeh, A. R.; Hashemi, S. M.; Gorab, M. G.; Maleki, A.; Cohan, R. A.; Mahdavi, M.; Poodat, R.; Keyvanlou, F.; Esmaeili, M. S. Recent advances on biomedical applications of pectin-containing biomaterials. Int. J. Biol. Macromol. 2022 , 217 , 1−18..

Li, X.; Zhang, L.; Liu, Z.; Wang, R.; Jiao, T. Recent progress in hydrogels combined with phototherapy for bacterial infection: a review. Int. J. Biol. Macromol. 2024 , 274 , 133375..

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