Optimizing　the　electronic　structure　of　the　surface　active　sites　and　introducing　functional　sites　for　a　photocatalyst　are　effective　strategies　to　achieve　the　photocatalytic　selective　hydrogenation　of　biomass.　Herein,　Pt　clusters/bimetallic　NiMg-MOF-74　(MNM)　ultrathin　nanosheets　were　constructed　for　the　photocatalytic　precise　hydrogenation　of　furfural　(FUR)　to　furfuryl　alcohol　(FAL).　A　representative　sample　(Pt/MNM-0.25)　shows　99.9%　conversion　of　FUR　and　99.9%　selectivity　of　FAL.　The　electron　density　of　surface　coordinatively　unsaturated　NiII　atoms　in　MNM　is　decreased　after　the　doping　of　Mg.　In　situ　ATR-IR　indicated　that　the　optimized　surface　NiII　sites　induced　a　more　effective　coordination　activation　of　FUR　molecules　via　the　Ni-η1-(O)-furfural　coordination.　Electrochemical　measurements　and　in　situ　EPR　results　reveal　that　Pt　clusters　are　the　functional　surface　sites　for　transferring　the　photogenerated　electrons　and　dissociating　H2.　The　synergistic　effect　of　surface　optimized　NiII　sites　and　Pt　clusters　is　emphasized.　This　work　successfully　achieves　the　high-efficiency　precise　hydrogenation　of　FUR　to　FAL　via　designing　surface　functionalized　Pt　clusters/bimetallic　MOF　ultrathin　nanosheets.　©　2023　Elsevier　B.V.