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Manganese‐based Na superionic conductors (NASICONs) Na4MnCr(PO4)3 with three‐electron reaction are attractive cathode materials for sodium‐ion batteries. However, the irreversible distortion of Mn local structure leads to sluggish electrode kinetics, voltage hysteresis, and poor cycling stability. Here, SiO4 is introduced to substitute PO4 to modulate the local environment of Mn to activate the redox...