Composition‐Driven Strain Self‐Organization for Stable Li‐Rich Cathodes

Lithium‐rich manganese‐based oxides (LRMOs) exhibit exceptional specific capacity owing to their unique combination of cationic and anionic redox activities, rendering them widely recognized as one of the most promising cathode materials for high‐energy‐density lithium‐ion batteries. However, their cycling stability is severely compromised by structural degradation arising from coupled electrochemical‐mechanical effects, including oxygen release, transition metal migration, and cumulative lattice strain upon repeated (de)lithiation cycles. Herein, a composition‐driven strain self‐organization strategy is proposed for LRMOs, conceptually inspired by the strain‐buffering function of the mortar layers in nacre. By establishing a periodic alternation of tensile and compressive regions, the strain‐buffering corrugation is constructed. Such an architecture effectively absorbs volume strain through cooperative microregional deformation, while the associated reversible dislocation evolution serves to avoid the accumulation of irreversible plastic strain. As a result, the structural reversibility and electrochemical performance in the modified LRMO are significantly improved. This work introduces a strain architecture design that imparts the superior mechanical features of natural nacre to electrochemical energy storage materials, opening a new avenue for the rational design of high‐stability Li‐rich Mn‐based cathodes.