Electrodeposition of FeCoNiCu/Cu nanometric, compositionally modulated alloy nanowires is presented. Pure Cu nanowires and Co-rich FeCoNiCu alloy nanowires were deposited from a single electrolyte. A double potential pulse scheme was used for multilayer deposition and significant anodic dissolution was observed during the low potential pulse. Galvanostatic triple pulses with a relaxation period were developed to minimize the local pH rise inside the nanopores during fabrication of the layered FeCoNiCu/Cu nanowires.