Interface Engineering for Heightening Anionic Redox Reversibility of Li‐Rich Layered Oxides Cathodes: Recent Advances and Perspectives

ABSTRACT Lithium‐rich manganese‐based layered oxides (LRMOs) are leading candidates for next‐generation high‐energy‐density lithium‐ion batteries, offering exceptional specific capacities exceeding 250 mAh g −1 . However, interfacial instability and surface structural degradation impede their commercial deployment. Current research lacks comprehensive analysis of dynamic interfacial mechanisms governing oxygen redox and corresponding engineering strategies. This review focuses on recent advancements in interface engineering to enhance the reversibility of anionic redox reactions in LRMOs, providing crucial insights for designing high‐performance batteries. The LRMO crystal structure, oxygen redox mechanism, and associated challenges are first outlined. Subsequently, we examine interfacial design progress including surface engineering, surface defect regulation, integrated modifications, and electrolyte engineering, highlighting how these approaches improve oxygen redox reversibility to mitigate the performance decline of LRMOs. Additionally, the mechanical and chemical instability mechanisms of all‐solid‐state battery interfaces and corresponding interface design strategies are discussed. Finally, we provide further insights and new perspectives for the better development of LRMO cathode materials.