Gradient Porous Elastic Hydrogels with Shape‐Memory Property and Anisotropic Responses for Programmable Locomotion

Programmable locomotion of responsive hydrogels has gained increasing attention for potential applications in soft robotics, microfluidic components, actuators, and artificial muscle. Modulation of hydrogel pore structures is essential for tailoring their mechanical strength, response speeds, and motion behaviors. Conventional methods forming hydrogels with homogeneous or stepwise‐distributed pore structures are limited by the required compromise to simultaneously optimize these aspects. Here, a heterobifunctional crosslinker enabled hydrothermal process is introduced to synthesize responsive hydrogels with well‐defined gradient pore construction. According to gradient porosity controls, the hydrogels simultaneously exhibit rapid responses to external stimuli, high elasticity/compressibility, and programmable locomotion capability. By incorporating polypyrrole nanoparticles as photothermal transducers, photo/thermal responsive composite hydrogels are formed to enable programmable control of locomotion such as bending, curving, twisting, and octopus‐like swimming under near‐infrared laser stimulation. The tunable pore structures, mechanical properties, and locomotion of this new class of materials make these gradient porous hydrogels potentially suitable for a variety of applications.