The Pt/(Fe, Mn/Co)-BTC catalysts were fabricated by a facile ultrasonic impregnation assisted hydrothermal polyol reduction method using first MIL-100(Fe, Mn/Co) MOFs as supports and tested for selective hydrogenation of furfural (FAL) to furfuryl alcohol (FOL). Various characterizations including XRD, TG, FT-IR, N-2 physical adsorption, ICP-OES, SEM, TEM and XPS were applied for exploring structure changes and surface properties of the catalysts. Over 98% conversion of FAL and 99% selectivity to FOL were achieved over Pt/(Fe, Mn)-BTC and Pt/(Fe, Co)-BTC, moreover, Pt/(Fe, Co)-BTC showed higher turnover frequency (TOF) of 1,044 h(-1) and better cycle stability, which are better than other catalysts prepared by using H-2, NaBH4, and formaldehyde as reductants. Overall, the formation of highly dispersed small-sized Pt NPs (about 1.7 nm) with much higher content of surface Pt-0 on the catalysts is the key of excellent hydrogenation activity due to the strong interaction between Pt NPs and the bimetallic supports.