Introducing hydrophilic PVP and sulfur vacancy into MoS 2 nanosheets boosts the photocatalytic Cr(VI) removal and antibacterial activity through adsorption and catalytic effects. [Display omitted] The exploration of novel nanomaterials to resolve the issues of water pollution with the aid of photocatalytic technology has always been a research hotspot. MoS 2 is acknowledged to be one of the promising photocatalysts for its interesting layered structure, suitable band gap, and good chemical stability. However, the fast recombination of photogenerated electrons and holes within the MoS 2 impedes its extensive application. Here, hydrophilic polymer (polyvinyl pyrrolidone, PVP) and sulfur vacancy (Vs) are simultaneously introduced into the MoS 2 nanosheets to achieve high-efficient photocatalytic hexavalent chromium Cr(VI) removal and antibacterial performance. The incorporation of PVP greatly enhances the adsorption capacity of MoS 2 , and creating Vs essentially strengthens the photogenerated carrier separation of MoS 2. As a result, the Cr(VI) removal efficiency of MoS 2 -PVP with an appropriate Vs concentration is up to 99.5 % for 3 h. Meanwhile, MoS 2 -PVP with a relatively higher Vs concentration displays a superior Escherichia coli (E. coli) removal efficiency of 91.8 % within 30 min with the initial E. coli concentration of ∼1.0 × 107 CFU/mL. This study extends photocatalysts to a higher level in designing advanced materials for environmental remediation and establishes a feasible platform for emphasizing the versatility of defect engineering in regulating catalytic activity. [ABSTRACT FROM AUTHOR]