Developing high-performance electrocatalysts toward hydrogen evolution reaction (HER) is important for clean and sustainable hydrogen energy, yet still challenging. Herein, an α-MoC 1 - x induced redispersing strategy to construct a superior HER electrocatalyst (Pt/CNTs-N + α-MoC 1 - x ) by mechanical mixing of α-MoC 1 - x with Pt/CNTs-N followed by thermal reduction is reported. It is found that thermo-activation treatment enables partial Pt atoms to redisperse on α-MoC 1 - x substrate from carbon nanotubes, which creates dual active interfaces of Pt species dispersed over carbon nanotubes and α-MoC 1 - x . Benefiting from the strong electronic interaction between the Pt atom and α-MoC 1 - x , the utilization efficiency of the Pt atom and the zero-valence state of Pt is evidently enhanced. Consequently, Pt/CNTs-N + α-MoC 1 - x catalyst exhibits excellent HER activity with low overpotentials of 17 and 34 mV to achieve a current density of 10 mA cm -2 in acidic and alkaline electrolytes, respectively. Density functional theory calculations further reveal that the synergistic effect between Pt and α-MoC 1 - x makes it accessible for the dissociation of water molecules and subsequent desorption of hydrogen atoms. This work reveals the crucial roles of α-MoC 1 - x additives, providing practical solutions to enhance platinum dispersion, and thereby enhance the catalytic activity in HER.