Skin‐Inspired All‐Natural Biogel for Bioadhesive Interface

Abstract Natural material‐based hydrogels are considered ideal candidates for constructing robust bio‐interfaces due to their environmentally sustainable nature and biocompatibility. However, these hydrogels often encounter limitations such as weak mechanical strength, low water resistance, and poor ionic conductivity. Here, inspired by the role of natural moisturizing factor (NMF) in skin, a straightforward yet versatile strategy is proposed for fabricating all‐natural ionic biogels that exhibit high resilience, ionic conductivity, resistance to dehydration, and complete degradability, without necessitating any chemical modification. A well‐balanced combination of gelatin and sodium pyrrolidone carboxylic acid (an NMF compound) gives rise to a significant enhancement in the mechanical strength, ionic conductivity, and water retention capacity of the biogel compared to pure gelatin hydrogel. The biogel manifests temperature‐controlled reversible fluid‐gel transition properties attributed to the triple‐helix junctions of gelatin, which enables in situ gelation on diverse substrates, thereby ensuring conformal contact and dynamic compliance with curved surfaces. Due to its salutary properties, the biogel can serve as an effective and biocompatible interface for high‐quality and long‐term electrophysiological signal recording. These findings provide a general and scalable approach for designing natural material‐based hydrogels with tailored functionalities to meet diverse application needs.