Fabrication of high-performance and low-cost metal-based compounds as electrocatalysts by a simple strategy is crucial for the hydrogen evolution reaction (HER). In this study, MnS-MoS 2 nanosheets were in situ grown on a laser-ablated Mo plate (MnS-MoS 2 /LA-Mo) through a one-step hydrothermal method. Benefiting from the high electrochemical activity area, good electrical conductivity, superhydrophilic/aerophobic surfaces, and ultrathin nanosheets, MnS-MoS 2 /LA-Mo exhibits excellent electrocatalytic activity and structure stability, delivering a low overpotential of 85 mV in a 0.5 M H 2 SO 4 electrolyte and 176 mV in a 1 M KOH electrolyte, respectively, at the current density of 10 mA cm −2 , exhibiting low charge-transfer resistance and exceptional long-term stability. This work provides a simple method for preparing efficient self-supporting nonprecious metal electrocatalysts.