While fuel cells are a promising technology for portable energy conversion, their incorporation into the energy infrastructure is impeded by significant materials issues. The primary issues with the anode catalyst are degradation and slow fuel oxidation kinetics, particularly for direct alcohol fuel cells. This dissertation explains many aspects of a large-scale research project focussed at identifying superior anode catalyst materials. Effective searching of the astronomical number of possible catalysts is achieved through the study of composition spread thin films. A high-throughput electrochemical fluorescence assay is used to evaluate the catalytic activity of the thin films and comparison of these measurements with detailed characterization of the thin film properties is used to establish trends that guide the choice of new materials. The developed characterization methods include the modeling and subsequent calculation of film composition and high-throughput mapping of crystallographic properties with high energy diffraction. Several new catalyst systems are presented, and the ensemble of techniques is also applied to known catalyst systems and shown to reveal important material properties.