Hydration Programmable, Shape Memorable Artificial Muscles for Antagonistic Movements

Abstract Shape memory polymers (SMPs) capable of generating various deformations from anisotropic temporary shapes to permanent shapes have been emerging as soft robots. However, traditional SMPs cannot imitate the antagonistic movement of human skeletal muscles due to their modulus limitations in shape programming and recovery process. Herein, hydration programmable shape memory polymer (HP‐SMP)‐based fibers that can undergo reversible actuation by assembling antagonistic pairs are reported, where the shape programming of the antagonist muscle relies on the contraction of agonist muscle. HP‐SMP fibers are composed of tunicate cellulose nanocrystals (TCNCs) reinforced semi‐interpenetrating polymer networks. Leveraging their distinctive structure and hydration programmability, the HP‐SMP fibers exhibit large actuation strain (−60%) and high work capacity (751 J kg⁻¹), allowing for reversible actuation under constant stress. Most significantly, the continuous antagonistic movements of HP‐SMP fibers assembled into artificial limbs are demonstrated to realize humanoid motion. This work provides new possibilities for replicating a series of lifelike human movements through the biomimetic design of antagonistic pairs of artificial muscles, utilizing renewable and sustainable biosourced materials.