Bimetallic catalysts are gaining flourishing research interest due to their tunable electronic and geometric structure over monometallic catalysts. Herein, we prepare a series of Pt–Sn nanoparticles with various Sn/Pt ratios encapsulated in an amine-functionalized Zr metal–organic framework (Pt–Sn@UiO-66-NH₂) by a sequential impregnation/reduction strategy. We find that PtSn_0.10@UiO-66-NH₂ with only 10% Sn addition significantly improves activity, selectivity, and stability toward the gas-phase furfural hydrogenation reaction compared with Pt@UiO-66-NH₂. By comparing the spectroscopic and the catalytic results of Pt and PtSn_0.10 nanoparticles confined in UiO-66 and UiO-66-NH₂, we find that the enhanced catalytic property of PtSn_0.10@UiO-66-NH₂ is ascribed to the triple synergistic effect among the Pt, Sn, and −NH₂ group on the MOF.