A　pile　of　unique　grain　boundary-engineered　ZnS(en)(0.5)　nanosheets　(D-ZnS(en)(0.5)　NSs)　are　constructed　via　a　solvothermal　process.　Large　amounts　of　stacking　fault　and　dislocation　in　D-ZnS(en)(0.5)　at　the　boundaries　could　create　mid-gap　defect　states,　in　which　intraband　transition　and　carrier　creation　are　induced　under　visible　light　irradiation.　Meanwhile,　a　defect-rich　structure　with　a　quasiperiodic　configuration　endows　the　integrated　polycrystalline　NSs　with　preferable　electrical　properties.　Owing　to　the　enriched　defect-state　excitation　and　optimized　electrical　properties,　D-ZnS(en)(0.5)　exhibits　superior　visible-light-driven　photocatalytic　performance　for　hydrogen　evolution　from　water.　This　work　will　provide　a　new　strategy　for　achieving　a　visible-light　organic-inorganic　hybrid　photocatalyst.