A series of Vulcan carbon-supported Pd-Cu catalysts with various molar ratios of Pd to Cu was prepared by co-impregnation followed by a reduction in a hydrogen atmosphere at three different temperatures. The degree of alloying between the two metals, alloy composition, and particle size and size distribution were characterized by X-ray diffraction, transmission electron microscopy, and energy-dispersive X-ray spectroscopy. The electrocatalytic activity for the oxygen reduction reaction (ORR) for these various compositions was determined using the thin-film rotating disk electrode technique. Our study reveals that the Pd-Cu bimetallic electrocatalysts, with a suitable degree of alloying, offer a greatly enhanced ORR activity compared to the Pd monometallic electrocatalyst. The best electrocatalytic activities were observed for the bimetallic catalysts that showed alloy nanoparticles with a Pd-Cu molar ratio of approximately 1:1.