By annealing [Mn(phen)H2O][V2O6] (phen = 1,10‐phenanthroline) in the presence of graphite template, MnV2O4 /C microparticles are obtained, in which MnV2O4 particles with one‐layer or few‐layer coating of graphene are anchored on the graphite sheets. The optimal sample, MnV2O4(p)/C‐700 with a high carbon content (35.3 at. %) can deliver a large specific capacity of 410 mAh g−1 at 0.1 A g−1 with a high capacity retention of 94.3% over 1000 discharge/charge cycles at 20 A g−1 as cathode in zinc‐ion battery. Ex situ X‐ray diffraction, scanning electron microscopy, energy‐dispersive X‐ray spectra, as well as elemental mappings and X‐ray photoelectron spectroscopy of MnV2O4(p)/C‐700 discern the partial phase transformation mechanism of MnV2O4→Zn3(OH)2V2O7(H2O)2 during discharge/charge process. It is because the rich oxygen defects of MnV2O4 can improve electrical conductivity, favor the electron transfer from V→Mn/O, thus facilitate the binding of Zn2+, and the captured Zn2+ cannot be extracted, as evidenced by density functional theory calculations. Furthermore, it is found that O‐deficiency can capture the water shell from the hydrated Zn2+, then the dehydrated Zn2+ is easy to insert into MnV2O4 with lower migration barrier of Zn2+ (0.84 eV), leading to the structural reversibility of MnV2O4 in cycling test.
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