Improving efficiency and reducing overall cost are two key issues to the commercialization of fuel cell powered vehicles. Electrocatalysts play an important role, particularly in the cathode, where the oxygen reduction reaction is sluggish and the noble metal loading is relatively high. To discover less expensive and more active cathode catalysts, a novel combinatorial workflow has been developed to investigate alloy-based electrocatalysts. In addition to the discovery program, various synthesis technologies have been studied and developed to engineer nanoscale catalyst particles with controllable size, monodispersity, and microcomposition. The progress of these research activities is reported with particular attention focused on the activity-stability-composition relationship for a series of platinum-based metal alloys.