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Abstract Layered lithium‐rich manganese‐based oxide (LRMO) has the limitation of inevitable evolution of lattice oxygen release and layered structure transformation. Herein, a multilayer reconstruction strategy is applied to LRMO via facile pyrolysis of potassium Prussian blue. The multilayer interface is visually observed using an atomic‐resolution scanning transmission electron microscope and a high‐resolution transmission electron microscope. Combined with the electrochemical characterization, the redox of lattice oxygen is suppressed during the initial charging. In situ X‐ray diffraction and the high‐resolution transmission electron microscope demonstrate that the suppressed evolution of lattice oxygen eliminates the variation in the unit cell parameters during initial (de)lithiation, which further prevents lattice distortion during long cycling. As a result, the initial Coulombic efficiency of the modified LRMO is up to 87.31%, and the rate capacity and long‐term cycle stability also improved considerably. In this work, a facile surface reconstruction strategy is used to suppress vigorous anionic redox, which is expected to stimulate material design in high‐performance lithium ion batteries.