A secondary neutral mass spectrometric ͑SNMS͒ depth profile study of electrodeposited Co/Cu multilayers was performed. Depth profile measurements were performed both in the conventional way ͑i.e., starting the sputtering from the final deposit surface͒ and in the reverse manner ͑i.e., detaching the multilayers from the substrate and starting the analysis from the substrate side, which was very smooth as compared to the final deposit surface͒. The latter method could yield significantly larger intensity fluctuations in the SNMS spectra. Surface roughness data were measured with atomic force microscopy ͑AFM͒ for multilayers with different bilayer numbers but otherwise exhibiting the same layer structure as those used for the depth profiling. The experimental AFM surface roughness evolution was used to calculate the result of the depth profile measurements quantitatively. An excellent agreement was obtained between this calculation and the SNMS measurements. It was shown that the decrease in the intensity fluctuations during the depth profile analysis stems mainly from the increase in surface roughness of the samples studied, especially in the conventional sputtering mode. It was also concluded that the thickness fluctuation of the entire multilayer deposit and that of each layer are strongly correlated. DOI: 10.1149/1.3133182 .Nanoscale magnetic/nonmagnetic multilayers are in the forefront of materials research since the discovery of giant magnetoresistance ͑GMR͒ in these nanostructures.1,2 Multilayers are mostly produced by physical methods ͑evaporation, sputtering, and molecular beam epitaxy͒, some of them applying a fairly expensive high vacuum system. The feasibility of the electrodeposition of metallic magnetic/ nonmagnetic multilayers with GMR was demonstrated 3 a few years after the discovery of the phenomenon. Although electrodeposition has long been considered as a possible low cost alternative to the physical sample preparation techniques, the quality of the electrodeposited ͑ED͒ multilayers is still inferior to their physically produced analogs. The literature of the ED multilayer films with GMR amounts to some 140 papers, 4-6 but very little is known about why the sample quality, especially GMR, cannot achieve the properties of the samples prepared by physical methods.Although depth profile analysis is a very efficient tool for the characterization of element distribution and the interface quality of ED multilayer samples, only a few studies were published hitherto. Basile et al.7 studied the depth profile of ED Co/Cu sandwiches by Auger electron spectroscopy. They found that the observed interface width of approximately 20 nm is an inherent feature of the sample itself rather than the artifact of the sputtering method used for the depth profiling ͑although the sputtering also leads to some intermixing at a smaller depth scale 8,9 ͒. According to Tokarz et al., 10 the interface width of ED Cu͑200 nm͒/Ni͑200 nm͒ bilayers can also be estimated as being 20-30 nm, as shown by their secondary-ion mass spe...