Mussel‐Inspired Robust Self‐Healing Triboelectric Materials Enabled by Supramolecular Interactions and Nanoconfinement

ABSTRACT Biomass‐based self‐healing triboelectric materials are recognized for meeting the sustainability and reliability demands of flexible electronic sensors, playing an essential role in enhancing device durability and operational longevity. However, existing self‐healing biomass systems still face challenges in achieving synergistic enhancement of both mechanical properties and self‐healing efficiency. Inspired by the strong adhesion of mussel foot proteins, a robust, room‐temperature self‐healing, and recyclable biomass‐based triboelectric material has been developed through the synergistic coordination of supramolecular interactions (such as Fe 3+ ─catechol coordination bonds, hydrogen bonds, and π─π stacking) and nanoconfinement. The constructed nanonetwork was found to facilitate enhanced energy dissipation and accelerated dynamic bonds reorganization, resulting in a combination of superior mechanical properties and efficient self‐healing. The obtained material demonstrated a tensile strength of 30.95 MPa, a toughness of 100.77 MJ m −3 , and a remarkable self‐healing efficiency of 96.22%. A triboelectric tactile sensor fabricated from this material exhibited a rapid response of 14 ms, and when integrated with deep learning algorithms, achieved highly accurate identification of material types and surface textures. This work offers a promising approach for the development of bionic perception systems in complex environments.