Direct 4D printing of functionally graded hydrogel networks for biodegradable, untethered, and multimorphic soft robots

Abstract Recent advances in functionally graded additive manufacturing (FGAM) technology have enabled the seamless hybridization of multiple functionalities in a single structure. Soft robotics can become one of the largest beneficiaries of these advances, through the design of a facile four-dimensional (4D) FGAM process that can grant an intelligent stimuli-responsive mechanical functionality to the printed objects. Herein, we present a simple binder jetting approach for the 4D printing of functionally graded porous multi-materials (FGMM) by introducing rationally designed graded multiphase feeder beds. Compositionally graded cross-linking agents gradually form stable porous network structures within aqueous polymer particles, enabling programmable hygroscopic deformation without complex mechanical designs. Furthermore, a systematic bed design incorporating additional functional agents enables a multi-stimuli-responsive and untethered soft robot with stark stimulus selectivity. The biodegradability of the proposed 4D-printed soft robot further ensures the sustainability of our approach, with immediate degradation rates of 96.6% within 72 h. The proposed 4D printing concept for FGMMs can create new opportunities for intelligent and sustainable additive manufacturing in soft robotics.