Photoreduction　is　recognized　as　a　desirable　treatment　method　for　hexavalent　chromium　(Cr(VI)).　However,　it　has　been　limited　by　the　intermittent　solar　flux　and　limited　light　absorption.　In　this　work,　a　novel　Z-scheme　photocatalyst　combining　a　covalent　organic　framework　(COF)　with　Eu2+,　Dy3+　co-doped　Sr2MgSi2O7　(Sr2MgSi2O7:Eu2+,　Dy3+)　is　synthesized,　which　shows　the　high　spectral　conversion　efficiency　and　works　efficiently　in　both　light　irradiation　and　dark　for　Cr(VI)　reduction.　Sr2MgSi2O7:Eu2+,　Dy3+　serves　as　both　an　electron　transfer　station　and　active　sites　for　COF　molecule　activation,　thus　resulting　in　100%　photoreduction　of　Cr(VI)　(50　mL,　10　mg/L)　with　high　light　stability　and　over　1　h　dark　activity.　Moreover,　the　XPS　and　FT-IR　analyses　reveal　the　existence　of　functional　groups　(Si-OH　on　Sr2MgSi2O7:Eu2+,　Dy3+,　and　-NH-　on　COFTP-TTA)　on　the　composited　catalyst　as　active　sites　to　adsorb　the　resultant　Cr(III)　species,　demonstrating　a　synergistic　effect　for　total　Cr　removal.　This　work　provides　an　alternative　method　for　the　design　of　a　round-the-clock　photocatalyst　for　Cr(VI)　reduction,　allowing　a　versatile　solid　surface　activation　for　establishing　a　more　energy　efficient　and　robust　photocatalysis　process　for　Cr　pollution　cleaning.