Bioinspired Self‐Healing Polymers in Lithium‐Ion and Lithium Metal Batteries: A Comprehensive Review of Electrode and Electrolyte Designs

ABSTRACT The integration of bioinspired self‐healing polymers into lithium‐ion batteries (LIBs) has been recognized as a promising strategy to overcome critical challenges such as mechanical degradation, dendrite formation, interfacial instability, and limited cycling stability. In this review, recent progress in the design and application of self‐healing materials for both electrolytes and electrodes in LIBs is comprehensively examined. A range of self‐healing mechanisms—including supramolecular interactions, dynamic covalent bonding, and zwitterionic functionalities—has been investigated for their ability to restore structural integrity and maintain electrochemical performance under operational stress. Various classes of polymer electrolytes are discussed, including supramolecular, zwitterionic, single‐ion conducting, gel‐based, and imine‐functional systems, with emphasis placed on their healing efficiencies, ionic conductivities, and compatibility with lithium metal. Electrode‐side strategies are also explored, covering gel‐based electrodes, silicon anode binders, and liquid metal anodes, where self‐repair is utilized to mitigate the effects of volume change, cracking, and structural fatigue. Key studies are highlighted, and performance trade‐offs are critically assessed. By providing a systematic evaluation of current strategies and their limitations, this review aims to inform the rational design of next‐generation LIBs with enhanced durability, safety, and functional longevity through the incorporation of intelligent, self‐healing materials.