ABSTRACTA variety of Cu/(Ni, Co) multilayers have been grown on Cu single crystals by pulse plating from an alloy electroplating bath. Copper is deposited under mass transport control while the iron group metal is deposited under interfacial charge transfer control. The structural evolution of these films is influenced by the morphological instability of the mass transport limited copper deposition reaction and the development of growth twins during iron-group metal deposition. Specular films have been obtained for growth on Cu(100) while rough, defective films were typically obtained for growth on Cu(111) and Cu(110).