Synergistic, Biomass‐Enhanced Hydrogels for Sustainable, All‐in‐One Sensing and Energy‐Autonomous Bioelectronics

ABSTRACT The development of multifunctional, sustainable material platforms that simultaneously deliver high performance, environmental adaptability, and integrated functionality remains a grand challenge in wearable electronics. Herein, we report a fully biomass‐enhanced conductive hydrogel engineered via a synergistic interplay between lignosulfonate (LS) and carboxymethyl cellulose (CMC) within a poly(AAm‐co‐DMC) network. This design leverages a hierarchical architecture of covalent cross‐linking and dynamic noncovalent interactions (electrostatic, hydrogen bonding, and π‐π stacking) to decouple the classic trade‐offs between mechanical robustness, functional versatility, and sustainability. The resultant material exhibits an exceptional combination of properties: remarkable mechanical robustness, rapid self‐healing, strong adhesion, and all‐weather operational stability enabled by an anti‐freezing ionic matrix. More importantly, this integrated functionality enables the hydrogel to serve as a unified, all‐in‐one platform capable of functioning as an ultra‐wide‐range strain sensor, a high‐fidelity electrode for electrophysiological monitoring, a high‐output triboelectric nanogenerator (TENG), and a stable supercapacitor (SC) electrolyte. Furthermore, an intelligent gesture recognition platform based on the collected electromyography signals, empowered by advanced machine learning algorithms, was developed to facilitate barrier‐free communication. This work establishes a sustainable design paradigm, demonstrating that the synergistic use of natural polymers can pave the way for next‐generation, energy‐autonomous wearable systems that are both high‐performing and environmentally benign.