Considering the practical use of electrochemical water splitting, it is important to construct a highly efficient and stable hydrogen evolution reaction (HER) electrocatalyst over a wide pH range. Herein, we develop an efficient strategy to enhance the electrochemical activity of few-layer MoS₂ and Pt nanoparticles (NPs) anchored on multi-wall carbon nanotube (MWCNTs). The as-prepared Pt-MoS₂/MWCNTs provides an excellent HER electrocatalytic activity with low overpotentials at −10 mA cm⁻² over a wide pH range, namely, 20 mV in 0.5 M H₂SO₄, 92 mV in 1.0 M phosphate buffer solution (PBS), and 75 mV in 1.0 M KOH, respectively. In addition, Pt-MoS₂/MWCNTs deliver the highest mass activity at the overpotential of 0.05 V, which is 8.1, 2.3, and 26.5 times higher than that of commercial 20 wt% Pt/C in acidic, neutral and alkaline media, respectively. Density functional theory (DFT) calculations revealed that the co-existence of MoS₂ and Pt NPs facilitated the water dissociation reaction and hydrogen generation, thereby enhancing the activity of HER. This work provides a potential strategy to construct high-performance electrocatalysts for HER over the entire pH range.