Spatial patterning of hierarchical lamellar-cellular structured hydrogels for programmable deformation-coupled information encryption

Inspired by organisms capable of adaptive morphological regulation, hydrogel actuators with softness and large deformability are attractive for biomedical devices and information encryption, yet remain limited by the lack of hierarchically oriented structures simultaneously enabling rapid actuation and high-order complex deformation. Here, we report a multiscale lamellar-confined assembly polymerization strategy for fabricating synchronous programmable shape-morphing and information-encoding hydrogels with hierarchically periodic lamellar-cellular structure. Owing to the periodic asymmetric stresses that amplify deformation and hierarchical porous channels that accelerate water transport, the obtained hydrogel exhibits large three-dimensional deformation with the rapidest recovery speed of 112.5°/s among the reported thermo-responsive hydrogels, facilitating programmable shape morphing by orchestrating localized curvature. Furthermore, a spatial orientation-patterning strategy is developed to precisely regulate the site-specific arrangement of lamellar-cellular structures for diverse cooperative sophisticated deformations at high speed. Importantly, the highly oriented architecture endows the hydrogel with tunable birefringence, enabling a dynamic encryption platform that couples programmable deformation with information encoding. This work provides a flexible structural strategy for preparing hydrogels with biomimetic dynamic information encryption. Hydrogel actuators have potential in a range of applications, but combining rapid actuation and complex deformation is challenging. Here, the authors report a lamellar confined assembly polymerisation strategy for preparing programmable shape-morphing and information-encoding hydrogels.