The effect of ion irradiation on the activation and conductivity of the basal plane of 2H-phase WS₂ remains elusive for the enhancement of hydrogen evolution reaction (HER) properties. The objective of this study is to increase the number of electrocatalytic active sites by creating multi-vacancies (W vacancy, S vacancy, or the coexistence of W and S vacancies), simultaneously combing with doping strategy to improve the intrinsic conductivity and activate the HER catalytic performance of S sites in the basal plane of pristine WS₂ nanospheres. Herein, high-energy Fe¹³⁺-ion irradiation technology was used to irradiate the WS₂ surface, which not only regulates multi-vacancies, but also introduces Fe dopants with Fe²⁺ and Fe³⁺ into WS₂. Density functional theory firstly demonstrates that the creation of multi-vacancies coupling with Fe doping could significantly narrow the band gap of pristine WS₂, which is beneficial to the acceleration of electron transfer during the HER process. Experimentally, moderate doses of the Fe¹³⁺-ion irradiated WS₂ electrocatalyst (8*10¹³) achieved the optimum HER activity with a higher current density, lower onset overpotential and excellent stability in acidic electrolyte. This strategy is a promising perspective for the design of highly efficient electrocatalysts via the Fe¹³⁺-ion irradiation pathway.