The giant magnetoresistance (GMR) was investigated for electrodeposited Co/Cu multilayers. In order to better understand the formation of individual layers and their influence on GMR, multilayers produced by two different deposition strategies were compared. One series of Co(2 nm)/Cu(t(Cu)) multilayers with t(Cu) ranging from 0.5 nm to 6 nm was produced with the conventional two-pulse plating by using a galvanostatic/potentiostatic (G/P) pulse combination for the magnetic/non-magnetic layer deposition, respectively, whereby the Cu layer deposition was carried out at the electrochemically optimized potential. Another Co(2 nm)/Cu(t(Cu)) multilayer series with the same t(Cu) range was prepared with the help of a G/P/G pulse combination. In this latter case, first a bilayer of Co(2 nm)/Cu(6 nm) was deposited in each cycle as in the G/P mode after which a third G pulse was applied with a small anodic current to dissolve part of the 6 nm thick Cu layer in order to ensure the targeted t(Cu) value. The comparison of the two series revealed that the G/P/G pulse combination yields multilayers for which GMR can be obtained even at such low nominal Cu layer thicknesses where G/P multilayers already exhibit bulk-like anisotropic magnetoresistance only. Surface roughness measurements by atomic force microscopy revealed that the two kinds of pulse combination yield different surface roughness values which correlate with the structural quality of the multilayers as indicated by the absence or presence of multilayer satellite reflections in the X-ray diffraction patterns. A separation of the superparamagnetic (SPM) contribution from the total observed GMR provided useful hints at the understanding of differences in layer formation between samples prepared with the two kinds of pulse combination. The results of multilayer chemical analysis revealed that mainly an increased Cu content of the magnetic layer is responsible for the onset of SPM regions in the form of Co segregations in the G/P/G multilayers with small Cu layer thicknesses. Magnetization measurements provided coercive force and remanence data which gave further support for the above interpretation of the GMR data. (C) The Author(s) 2014. Published by ECS. All rights reserved.