The results of controlling the preferential crystallographic orientation of electrodeposited Ni-Cu multilayers by means of electrochemical methods are reported. These multilayers were grown on pulse electrodeposited and de electrodeposited copper foils of (111) and (220) preferential crystallographic orientation, respectively Since multilayers have a tendency to grow epitaxially, the multilayers grown on these substrates exhibited (111) or (220) preferential crystallographic orientation. Results of electrodeposition of multilayers on cold-rolled copper foil and on titanium are also presented. Similar results can be obtained using polycrystalline copper foil as compared to single crystal copper substrates.