Robust and Tough Recyclable C‐lignin‐Based Triboelectric Materials Enabled by Nano‐Confinement and Solvent‐Induced Effects

Abstract Developing biomass‐based triboelectric films with excellent robust and superior tough is crucial for realizing next‐generation green, sustainable and flexible wearable sensors. However, simultaneously achieving highly robust and superior tough in biomass‐based triboelectric films remains a significant challenge. In this study, inspired by natural creatures, particularly spider silk, based on the structural properties of catechol lignin (C‐lignin, CL) and the synergistic effects of nano‐confinement and solvent‐induced, the robust and tough recyclable C‐lignin‐based triboelectric films (CNT/CL/PVA film, CCLPF) with a multi‐scale reinforcement network was successfully constructed. The prepared lignin‐based films exhibited high tensile strength (43.1 MPa, 816%), excellent fracture toughness (512.3 MJ m ⁻³ ), outstanding energy dissipation efficiency (94.9%), superior antibacterial properties, significant antioxidant capacity, and stable triboelectric output performance (245.1 V and 7500 cycles). Notably, a self‐powered sensor array is also designed that could accurately perceive pressure distribution changes of different objects, thereby meeting diverse application demands and ultimately providing important technical pathways for the development of wearable devices and human‐machine interaction systems. In summary, this study not only offers a novel solution to the conflict between robust and tough in biomass‐based triboelectric films but also opens new avenues for the extensive application of lignin resources in flexible electronics and self‐powered sensing technologies.