Introducing anion vacancies on two-dimensional transition-metal dichalcogenides (TMDs) would significantly improve their catalytic activity. In this work, we proposed a solid-phase reduction (SPR) strategy to simultaneously achieve efficient exfoliation and controlled generation of chalcogen vacancies on TMDs. Consecutive sulfur vacancies were successfully created on the basal plane of the bulk MoS2 and WS2, and their interlamellar distances were distinctly expanded after the SPR treatment (about 16%), which can be conveniently exfoliated by only gentle shaking. The S-vacancy significantly increases the hydrogen-evolution reaction activity of the MoS2 and WS2 nanosheets, with overpotential of -238 and -241 mV at 10 mA cm-2, respectively. We anticipate that our SPR strategy will supply a general platform for the development of TMD-based electrocatalysts for industrial water splitting and hydrogen production in the near future.