Ni-based chalcogenide catalysts show the weak H2O molecule adsorption and sluggish kinetics, restricting their industrial hydrogen evolution reaction (HER) in a wide pH range. Herein, a controllable fabrication strategy of NiS/NiCoP nanoparticles by simultaneously constructing sulfur vacancies and introducing the heterometallic atoms (Zn, Fe, Mn) (M-NiCoSP-Sv) is proposed. The numerous uncoordinated surface Ni centers generated by sulfur vacancies are beneficial for cleaving the HO–H bond of H2O molecule, while S sites at Sv-NiS side and P sites at Zn-NiCoP side with rich electron aggregation are used as H2-evolution centers, synergistically facilitating HER kinetics over a wide pH range. As respected, Zn-NiCoSP-Sv exhibits excellent durability and outstanding HER activity such as 41, 78 and 34 mV of 10 mA cm–2 in alkaline, neutral and acidic electrolytes, respectively. And at the industrial current density, Zn-NiCoSP-Sv also possesses outstanding HER activity and stability. This work reveals a strategy for activating NiS-based catalyst to cleave H2O and optimize Gibbs free energy of H* by vacancy and doping co-engineering.