A series of platinum-coated underlayer materials, alumina, gold, titanium carbide, and titanium disilicide, deposited by a high throughput magnetron sputtering method have been investigated as cathode catalyst supports in fuel cells. Orthogonal thickness gradients of the underlayer materials ͑0-100 nm planar equivalent͒ and the platinum top layer ͑0-75 nm planar equivalent͒ made up the 76 ϫ 76 mm libraries. The resulting catalyst films were characterized by surface profilometry, X-ray diffraction, scanning electron microscopy, and X-ray photoelectron spectroscopy. The electrochemical properties of the catalyst composition spreads were investigated simultaneously in 64-electrode proton exchange membrane fuel cells with emphasis placed on the determination of the electrochemical surface area ͑ECSA͒ as a function of underlayer thickness and chemistry. The present study shows that gold and titanium disilicide used as underlayers on 3M's nanostructured thin film supports lead to a loss of ECSA during operation. Migration and surface accumulation were observed when gold was used as underlayer material. For titanium disilicide, alloying and the generation of platinum silicide phases occurred. Alumina and titanium carbide were found to be potentially acceptable underlayer materials as well as alternative support materials on the basis of their influence on the catalyst surface area.Polymer electrolyte membrane fuel cells ͑PEMFCs͒ are promising power sources for automotive applications in the future. 1 The main environmental advantage of using PEMFCs in vehicles is the reduction of carbon dioxide emissions, pollutants, and consumption of fossil fuels. 2 To fully commercialize PEMFCs for automotive vehicles, their high production cost needs to be reduced while improving performance and durability. The core of a PEMFC, the membrane electrode assembly ͑MEA͒, consists of two electrocatalyst electrodes ͑anode and cathode͒ with gas diffusion layers ͑GDLs͒ on either side of the proton-conducting ion-exchange membrane. Each of these MEA components contributes to the overall performance, stability durability, robustness, and cost of a PEMFC, and thus research efforts have been focused on the improvement of the electrocatalyst and membrane properties. 3 Platinum or platinum alloys are commonly used as the catalyst on the anode side for the hydrogen oxidation reaction ͑HOR͒ and on the cathode side for the oxygen reduction reaction ͑ORR͒ in a PEMFC. These catalysts may consist of highly dispersed platinum particles ͑2-3 nm͒ supported on carbon blacks, activated carbon, or carbon nanotubes. A range of factors 4 are known to contribute to the significant performance degradation of PEMFCs that can occur during long-term operation or as a result of adverse operating conditions ͑e.g., fuel starvation on the anode side during start-up and shutdown 5 ͒. These include Pt-catalyzed corrosion of the carbon support, 6 oxidation and decomposition of the GDL, 7 dissolution or poisoning of the Pt catalysts on the cathode and anode side, 8 and degr...