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Recently, Mg‐ion batteries (MIBs) and Mg−Li hybrid ion batteries (MLIBs) are deemed as potential energy‐storage devices. However, due to the insufficient storage sites of Mg 2 + in the cathode, MIBs show a low reversible capacity. For MLIBs, the property is also seriously restricted due to the main Li + intercalation reaction and less Mg 2+ intercalation reaction. Herein, ultrathin MoSe 2 nanosheets with enriched atomic defects and exposed edge surfaces are prepared by the hydrothermal method and subsequent hydrogen treatment. It is found that the Mg 2+ storage performance is markedly enhanced, and Mg 2+ /Li + co‐intercalation can be achieved. Density functional theory (DFT) calculation shows that, by introducing a large number of atomic defects and edge exposed surfaces in the ultrathin MoSe 2 nanosheets, the Mg 2+ storage sites are increased, and the diffusion and migration ability of Mg 2+ and Li + are improved, resulting in a significant property improvement. Further, the Mg 2+ intercalation in MIBs and Mg 2+ /Li + co‐intercalation in MLIBs are confirmed. The discharge‐charge mechanisms only based on the intercalation reactions for both MIBs and MLIBs are also revealed.

Enhancing Mg2+ and Mg2+/Li+ Storage by Introducing Active Defect Sites and Edge Surfaces in MoSe2