The poor high-rate dischargeability of negative electrode materials (hydrogen storage alloys) has hindered applications of nickel metal hydride batteries in high-power fields, new-energy vehicles, power tools, military devices, etc. In this work, a new strategy is developed to improve the high-rate performance of hydrogen storage alloys by coating MoS2 nanosheets on alloy surfaces. The capacity retention rate of the composite electrode reaches 50.5% at a discharge current density of 3000 mA g−1, which is 2.7 times that of bare alloy (18.4%). The density functional theory simulations indicate that such an outstanding performance is derived from adjustments of ion concentrations at the electrode/electrolyte interface by MoS2 nanosheets: (1) the higher OH− concentration facilitates the electrochemical reaction of MHads + OH− − e− → M + H2O; and (2) the lower H+ concentration leads to a large gradient between the electrode/electrolyte interface and interior of alloys, which is beneficial for the diffusion of atomic hydrogen during the discharging process.