NiFe/Cu multilayers were deposited from a single bath in the potentiostatic mode using two different solutions. In solution A, the ionic concentration ratios were Fe2 :Ni2 :Cu2 9:60:10 and in solution B they were 1:103:1. To characterize the layers, scanning electron microscopy (SEM), high resolution transmission electron microscopy (HRTEM), X-ray diffraction (XRD) and atomic force microscopy (AFM) were used. SEM results revealed the layered structure of the deposits for relatively thick bilayers. While HRTEM provided direct evidence for the composition modulation across successive layers in the NiFe/Cu nanometer-multilayered structure prepared from solution B. Therefore, the layers prepared from solution B seemed to be more appropriate for giant magnetoresistance (GMR) applications. The effect of stirring during the electrodeposition process of the multilayers was also investigated.