Metal-nanoparticle (NP)/metal-organic framework (MOF) composites have attracted considerable attention as heterogeneous catalysts. Compared with porous carbon, silica, and alumina, the charge-transfer interaction between the metal NPs and the MOF accelerated the catalytic activity. In this study, PdRu bimetallic NPs were successfully immobilized on MOFs such as MIL-101(Cr) by using supercritical carbon dioxide. The STEM-EDX images show a uniform 3D distribution of the PdRu bimetallic NPs on MIL-101(Cr). The resulting PdRu@MIL-101(Cr) catalyst exhibited higher CO oxidation than monometal/MOF composites such as Pd@MIL-101(Cr) and Ru@MIL-101(Cr). Furthermore, PdRu@MIL-101(Cr) exhibited higher catalytic activity than PdRu@SiO2. This is because the particle size of the PdRu bimetallic NPs in MIL-101(Cr) was within the range of 2-3 nm. The synergistic effects were based on the combination of two metals, Pd and Ru, small bimetal particle formation, and charge-transfer interactions between the bimetal NPs and the MOF. These factors enhance the catalytic activity of the bimetal/MOF composites.