Self‐Evolving Hierarchical Hydrogel Fibers with Circadian Rhythms and Memory Functions

Abstract The fusion of hierarchical tissues at interfaces, incorporating ultrafast selective transport channels, enables efficient matter exchange and energy transfer across multiscale structures in living organisms. However, achieving these characteristics simultaneously in an artificial multimaterial system is challenging. Here, this work presents a multimaterial hydrogel fiber with a hierarchical structure of interface fusion, which forms spontaneously through in situ hierarchy evolution induced by ionic cross‐linking and molecular shear flow. Water transport occurs in the angstrom‐scale confined slits created by aligned cellulose nanocrystals (CNCs) by direct Coulomb knock‐on, resembling Newton's cradle motion. The fusion of interfaces enables high‐efficiency water transport across multiscale layers, combined with Newton's cradle‐like collective water motion, creating a highly sensitive negative feedback loop within the fiber. These fibers exhibit integrated behaviors of time‐space perception, short‐term memory and adaptive changes in shape. Additionally, they demonstrate rhythm characteristics, changing periodically in a 24‐h day‐night cycle. Composed of natural building blocks, these hierarchical hydrogel fibers exhibit a memristor effect similar to that of an elementary neuron, making them promising for applications in seamless on‐skin and implantable bioelectronics.