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 Ni^II atoms in MNM is decreased after the doping of Mg. In situ ATR-IR indicated that the optimized surface Ni^II 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 Ni^II 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.