Multilayer nanowires tailored with alternating AuFe porous layers and Au nonporous segments were fabricated by galvanic square-wave pulsed electrodeposition from a AuFe cyanide-free electrolyte. Control of porosity and composition was achieved via modulation in pulsed time and applied current density. Nanowires with decreased porosity were observed upon increasing time of the AuFe alloy layer or shifting the applied current density to more negative values. This transition was consistent with an increased amount of material being deposited. The single-step approach presented is less time-consuming than conventionally fabricated nanoporous materials, requiring additional etching of prefabricated solid alloys. (C) 2009 The Electrochemical Society. [DOI:10.1149/1.3238471] All rights reserved.