Cu-based, solid oxide fuel cell (SOFC) electrodes were modified by electrodeposition of Co. The addition of only 5-vol% Co by electrodeposition significantly improved the thermal stability compared to either Cu-ceria-YSZ, Cu-Co-ceria-YSZ, or Co-ceria-YSZ electrodes prepared only by impregnation with much higher metal loadings, demonstrating that electrodeposited metal layers form metal films with better connectivity. In the absence of Co, SEM showed structural changes in the impregnated Cu after heating to 1173 K in humidified H2 and these changes caused large increases in the ohmic resistance of fuel cells, as measured by impedance spectroscopy. In contrast, the ohmic resistance of a cell with 13-vol% Cu, 9-vol% ceria, and 5-vol% Co increased only slightly after 48 h at 1173 K in humidified H2. While a Co-ceria-YSZ composite was found to form large amounts of carbon upon exposure to dry CH4 at 1073 K for 3 h, the Co-Cu-ceria-YSZ composites did not form measurable amounts of carbon for the same conditions. XPS results for a Cu foil with a 250-nm Co film demonstrated that Cu migrates to the surface of the Co upon heating above 873 K, forming a stable Cu layer that appears to be approximately one monolayer thick. The implication of these results for the development of practical SOFC electrodes for the direct utilization of hydrocarbons is discussed.