The electrocatalytic activities of a wide range of ordered intermetallic phases toward a variety of potential fuels have been studied, and results have been compared to those of a pure polycrystalline platinum (Pt(pc)) electrode. A significant number of the ordered intermetallic phases exhibited enhanced electrocatalytic activity when compared to that of Pt, in terms of both oxidation onset potential and current density. The PtBi, PtIn, and PtPb ordered intermetallic phases appeared to be the most promising electrocatalysts tested thus far for fuel cell applications. PtPb, in particular, showed an onset potential that was 100 mV less positive and a peak current density approximately 40 times higher than those observed for Pt in the case of methanol oxidation. The ability to control the geometric and electronic structures of the electrocatalytic material by using ordered intermetallic phases has been shown to be a promising direction of inquiry in the search for superior electrocatalysts for fuel cell applications.