Bioinspired Ion‐Proton Bipathway All‐Natural Hydrogel With Enhanced Conductivity for Bioelectronic Interfaces

ABSTRACT Sustainably derived all‐natural conductive hydrogels offer a new class of soft materials with intrinsic biocompatibility, biodegradability, and tunable mechanical properties, showing great promise for flexible bioelectronic interfaces. However, their practical application remains limited by inherently low electrical conductivity. Ion channels in the human nervous system, composed of proteins and oligosaccharides, can reduce the effective radius of hydrated ions by inducing partial dehydration of the hydration shell, thereby enabling highly efficient and ordered ion‐proton cooperative transport. Inspired by this ability, an all‐natural highly conductive ion‐proton bipathway hydrogel (IPBH) composed of bovine serum albumin (BSA), chitosan oligosaccharide (COS), and Ca 2 + was developed to mimic natural ion transport environments and significantly enhance the conductivity. The resulting IPBH achieves a remarkable conductivity of 40.59 mS/cm, which is 1272% and 384% higher than that of the proton‐only and ion‐only conductive hydrogels, respectively. Besides, the IPBH exhibits complete biodegradability within 36 h and exceptional biocompatibility. Moreover, the IPBH exhibits excellent low‐noise performance in physiological signal monitoring, enabling accurate EMG‐based gesture recognition integrated with a convolutional neural network (CNN) model for real‐time robotic arm control. This synergistically conductive, ion‐proton coupled hydrogel provides a versatile and sustainable platform for next‐generation high‐performance bioelectronic interfaces.