Chain‐Dynamics‐Mediated Interfacial Wetting in Structurally Hydrophobic Active Hydrogels

ABSTRACT Adaptive interfaces enable the conversion and redistribution of interfacial energy into coordinated mechanical actuation and molecular transport. In most soft material systems, mechanical motion is driven by asymmetric interfacial energy gradients, whereas molecular transport is governed by bulk diffusion through the polymer network. However, these pathways for interfacial energy transduction are rarely governed by one unified physical mechanism and accessible simultaneously, thereby constraining multifunctional adaptability. Herein, we present a structurally hydrophobic active hydrogel that undergoes water‐induced polymer chain rearrangements, thereby generating a dynamic surface‐energy gradient. By harnessing the energy gradient, the active hydrogels achieve autonomous locomotion at water‐air interface without any external energy supply. In parallel, the same wetting‐mediated mechanism enables the active hydrogels to load and accommodate multi‐polarity molecules simultaneously. Leveraging the synergistic effect of multi‐drug loading, active hydrogels demonstrate simultaneous and sustained release of hydrophobic curcumin and hydrophilic methylene blue for 120 h, reaching cumulative release of 72.89% and 51.28%, respectively. The synergistic release profiles are regulated through compositions and external stimuli, thereby providing a more comprehensive strategy than monotherapy alone. These adaptive interfacial behaviors of active hydrogels, governed by a unified physical mechanism, offer a compatible and scalable route to realizing multifunctionality in a single‐material system.