| Summary: | The slow diffusion dynamics hinder aqueous MnO<sub>2</sub>/Zn batteries’ further development. Here, a Ni/Fe bimetallic co-doped MnO<sub>2</sub> (NFMO) cathode material was studied by density functional theory (DFT) calculation and experimental characterization techniques, such as cyclic voltammetry (CV), galvanostatic intermittent titration technique (GITT) and electrochemical impedance spectra (EIS). The results indicated that the energy band structure and electronic state of MnO<sub>2</sub> were effectively optimized due to the simultaneous incorporation of strongly electronegative Ni and Fe ions. Consequently, the NFMO cathode material exhibited a faster charge transfer and ion diffusion dynamics than MnO<sub>2</sub> (MO), thus, the assembled NFMO/Zn batteries delivered excellent rate performance (181 mA h g<sup>−1</sup> at 3 A g<sup>−1</sup>). The bimetallic ions co-doping strategy provides new directions for the development of oxide cathode materials towards high-performance aqueous zinc-ion batteries.
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