Catalytic hydrogenation of CO2 to valuable chemicals is one of the key technologies to relieve global warming and promote thesustainable development of human society. Two - dimensional MoS2 materials have emerged as promising catalysts for CO2 activationand conversion due to their unique layered structure and adjustable S vacancies sites, which is the key active center for CO2 hydrogenation.In order to develop an efficient process for S vacancy creation, building S vacancies on MoS2 nanosheet were used as the basis for introducing S vacan-cies on the surface using H2O2 etching method, and the reaction properties of CO2 at atmosphere and high pressure beforeand after H2O2 etching were compared. The results show that H2O2 etching can significantly enhance the content of S vacancies without changing the crystal structure of MoS2 or affecting the chemical properties of S vacancy sites, which significantly enhances the conversion rate of CO2 catalytic hydrogena-tion without affecting the product distribution. Specifically, the S vacancies catalyze CO2 dissociationto pro-duce CO at atmosphere pressure with selectivity higher than 96%, whereas they are able to catalyze the hy-drogenation of CO2 tothe methanol at high pressure of 5 MPa and 180 ℃ with high selectivity (79%). In-creasing the reaction temperature improves theCO2 conversion, but the selectivity of methanol will be signifi-cantly reduced, accompanied by the generation of methane. Briefly, thiswork demonstrates a simple and ef-fective method to create S vacancies on MoS2, providing theoretical and technical support for the industrial application of MoS2 catalysts.