The electrochemical deposition of Cu into 0.12 cm and 60 µm thick, highly porous 65 vol % Ni/yttria-stabilized zirconia (YSZ) cermets was investigated. An electrochemical cell in which the electrolyte solution was allowed to flow through a porous Ni/YSZ substrate was used to eliminate mass-transfer limitations and to determine the conditions for which the potential drop in the electrolyte solution was minimized and a uniform Cu layer was produced throughout the porous substrate. The conditions determined from these experiments were then used to electrodeposit Cu throughout a thin, porous Ni–YSZ cermet anode layer on a solid oxide fuel cell (SOFC) using a standard nonflow-through setup. This SOFC was found to exhibit stable operation while using methane as the fuel.