Electrochemically Driven Dissipative Growth of Affinity Hydrogels for Bioresponsive Interfaces

ABSTRACT Nature provides an extraordinary blueprint for materials that are dynamic, self‐regulating, and adaptive. In living systems, these capabilities arise from continuous energy consumption, structural reorganization, and feedback‐driven molecular recognition, enabling biological matter to evolve, respond to stimuli, and sustain functions over time. In contrast, synthetic materials, despite their precision‐engineered properties, remain largely static, lacking the ability to sense, adapt, or remodel themselves in changing environments. Bridging this gap by imparting life‐like adaptability to synthetic systems would mark a transformative advance for bioelectronics and biomedical engineering. Here, we introduce a biocompatible strategy for the dissipative growth and reinforcement of hydrogel films, powered by electrochemical energy. Coupling redox‐controlled disulfide chemistry with programmable voltage pulses enables temporally regulated hydrogel fabrication with enhanced mechanical properties and efficient integration of affinity ligands, such as aptamers. The resulting affinity hydrogels achieve dynamic capture and release of growth factors via hybridization‐driven binding and electrochemical modulation of the hydrogel stiffness. These findings pave the way for dynamic biointerfaces and adaptive bioelectronic devices capable of sensing and responding to complex biological environments.