The oleylamine thermal reduction process was employed to prepare bimetallic copper-silver (Cu x Ag (0 # x # 50)) nanoparticles, such as Cu, Cu 50 Ag, Cu 20 Ag, Cu 10 Ag, Cu 5 Ag, CuAg, CuAg 2 , and Ag, by using Cu(CH 3 COO) 2 and AgNO 3 as the precursors. The samples were characterized by X-ray diffraction, transmission electron microscopy, thermogravimetric analysis, and X-ray photoelectron spectroscopy. The Cu x Ag hybrid nanostructure showed good particle dispersion, and Cu and Ag metals were well mixed. The catalytic properties of these bimetallic Cu x Ag nanoparticles as model catalysts for the Rochow reaction were explored. Compared to monometallic Cu and Ag nanoparticles, bimetallic Cu x Ag nanoparticles resulted in a much higher silicon conversion, which is attributed to the synergistic electronic effect between Cu and Ag metals. For example, the Cu atom was observed to have a lower electron density in the Cu x Ag bimetallic nanoparticle than that in monometallic Cu nanoparticles, which enhanced the formation of methylchlorosilanes on the silicon surface with chloromethane, demonstrating the significance of the Cu x Ag bimetallic catalysts in catalytic reactions during organosilane synthesis. The insights gained in this study should be conducive to the design of good Cubased catalysts for the Rochow reaction.