Hierarchical crack-resistant, tissue-mimetic hydrogels enabled by progressive nanocrystallization of anisotropic polymer networks

Huamin Li, Haidi Wu, Cheng Guan, Wenjie Hu, Wenwen Su, Dingdong Chen and Jiefeng Gao ()
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Huamin Li: Yangzhou University, School of Chemistry and Materials
Haidi Wu: Yangzhou University, School of Chemistry and Materials
Cheng Guan: Yangzhou University, School of Chemistry and Materials
Wenjie Hu: Yangzhou University, School of Chemistry and Materials
Wenwen Su: Yangzhou University, School of Chemistry and Materials
Dingdong Chen: Yangzhou University, School of Chemistry and Materials
Jiefeng Gao: Yangzhou University, School of Chemistry and Materials

Nature Communications, 2025, vol. 16, issue 1, 1-14

Abstract: Abstract Addressing the persistent challenge of reconciling extreme mechanical robustness with tissue-mimetic functionality in hydrogels, we present a phase-transition-guided hierarchical engineering strategy that progressively architectures anisotropic polyvinyl alcohol networks through sequential mechanical training, wet-annealing, and salting-out. This triphasic processing induces programmable structural evolution: (1) mechanical training aligns polymer chains, (2) wet-annealing relaxes the stress while stabilizes oriented crystallites through solvent-plasticized rearrangement, and (3) salting-out densifies the network via chain aggregation and hydrogen-bond proliferation. The resultant hierarchical architecture achieves high fatigue resistance (threshold: 2083 J·m−2) through multi-scale energy dissipation: sacrificial hydrogen bonds consume energy, while aligned crystalline domains pin the crack and deflect crack propagation via anisotropic stress redistribution. Demonstrating tissue-surpassing mechanics (tensile strength: 61 ± 3 MPa, toughness: 106 ± 27 MJ·m−3, fracture energy: 85 ± 9 kJ m−2) coupled with biological functionality, the hydrogel directs cell alignment through contact guidance while resisting swelling-induced dimensional instability (

Date: 2025
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DOI: 10.1038/s41467-025-65917-3

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