Abstract
Stimuli-responsive shape-changing hydrogels are attractive candidates for use as underwater soft robots. The bottleneck lies in the low actuation speed inherently limited by the water diffusion between hydrogels and their surrounding environment. In addition, accessing complex motions is restricted by the material fabrication methods. Here we report a hitherto unknown mechanism to achieve high-speed and programmable actuations for a disulfide crosslinked thermally responsive hydrogel. The dynamic photo-activated disulfide bond exchange allows photo-mechanical programming to introduce spatio-selective network anisotropy. This gives rise to an actuation behavior dominated by thermally driven conformation change of the locally oriented polymer chains instead of the common mass-diffusion-based mechanism. With the incorporation of photothermal fillers, light-powered oscillation at frequencies as high as 1.7 Hz is realized. This, coupled with the versatility of the programming, allows access to robots with diverse high-speed motions including continuous swimming, step-wise walking, and rotating.