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Biomimetic Organohydrogels with Tunable Architectures via Controlled Evaporation–Freeze/Thaw Self-Assembly

Yong Liu,Kangjie Zhou,Zhuo Huang,Heng Luo,Zhengping Fang,Shuaiyuan Wang,Huiyu Yang,Hai Liu

Conventional hydrogels often face inherent limitations such as dehydration sensitivity, mechanical brittleness, and optical opacity, which severely restrict their advanced applications. In this study, we report a controlled evaporation–freeze/thaw self-assembly strategy for fabricating biomimetic poly(vinyl alcohol)/graphene oxide nanosheet (PG) organohydrogels with tunable architectures. Inspired by natural nacre, homogeneous layered PG organohydrogels are engineered to simultaneously achieve superior mechanical properties and optical transparency, enabled by a nacre-mimetic “brick-and-mortar” microstructure with aligned polymer–nanosheet interfaces. Remarkably, post-treatments combining prolonged evaporation and UV-induced reduction synergistically enhance the mechanical performance, yielding a tensile strength of 6.3 MPa and toughness of 43.0 MJ/m3, surpassing those of many reported poly(vinyl alcohol) (PVA)-based hydrogels. Furthermore, the humidity-regulated self-assembly process enables the creation of skin-like gradient PG organohydrogels, mimicking epidermal–dermal structural hierarchies to achieve optimized water retention and mechanical stability. This work establishes a universal platform for designing high-performance hydrogels that reconcile traditionally conflicting properties, offering great potential for applications in flexible electronics, soft robotics, and biointegrated devices that require environmental adaptability.