Structural engineering of the molybdenum disulfide (MoS 2 ) retains its importance for the application of the hydrogen evolution reaction (HER) in a full pH range. However, the catalytic performance of reported MoS 2 -based materials, especially in neutral conditions, is unsatisfactory. Herein, an effective synergy between CoP, Ni 2 P, and MoS 2 nanosheets is established via a simple strategy, which constructs a self-supporting (CoP/Ni 2 P/MoS 2 −CC) electrode endowed with abundant catalytic active sites, optimal electronic structure, and improved charge transfer capability. The optimized CoP/Ni 2 P/MoS 2 −CC sample shows low overpotentials of 335, 119, and 211 mV at 100 mA cm −2 in neutral, alkaline, and acidic electrolytes with small Tafel slopes of 63, 62, and 82 mV dec −1 , respectively. Remarkably, the catalytic performance in neutral medium is superior to that of most of the reported MoS 2 -based hybrid electrocatalysts. Our work proves a facile and feasible strategy to promote the pH-universal catalytic activities of MoS 2 -based heterogeneous structures for hydrogen production.