The giant magnetoresistance (GMR) and structure was investigated for electrodeposited Co/Cu multilayers prepared by a conventional galvanostatic/potentiostatic pulse combination from a pure sulfate electrolyte with various layer thicknesses, total multilayer thickness and Cu deposition potential. X-ray diffraction (XRD) measurements revealed superlattice satellite reflections for many of the multilayers having sufficiently large thickness (at least 2 nm) of both constituent layers. The bilayer repeats derived from the positions of the visible superlattice reflections were typically 10 - 20% higher than the nominal values. The observed GMR was found to be dominated by the multilayer-like ferromagnetic (FM) contribution even for multilayers without visible superlattice satellites. There was always also a modest superparamagnetic (SPM) contribution to the GMR and this term was the largest for multilayers with very thin (0.5 nm) magnetic layers containing apparently a small amount of magnetically decoupled SPM regions. No oscillatory GMR behavior with spacer thickness was observed at any magnetic layer thickness. The saturation of the coercivity as measured by the peak position of the MR(H) curves indicated a complete decoupling of magnetic layers for large spacer thicknesses. The GMR increased with total multilayer thickness which could be ascribed to an increasing SPM contribution to the GMR due to an increasing surface roughness, also indicated by the increasing coercivity. For multilayers with Cu layers deposited at more and more positive potentials, the GMR(FM) term increased and the GMR(SPM) term decreased. At the same time, a corresponding reduction of surface roughness measured with atomic force microscopy indicated an improvement of the multilayer structural quality which was, however, not accompanied by an increase of the superlattice reflection intensities. The present results underline that whereas the structural quality as characterized by the surface roughness generally correlates fairly well with the magnitude of the GMR, the microstructural features determining the amplitude of superlattice reflections apparently do not have a direct influence on the GMR. (C) The Author(s) 2015. Published by ECS. This is an open access article distributed under the terms of the Creative Commons Attribution Non-Commercial No Derivatives 4.0 License (CC BY-NC-ND, Intp://creativecommons.org/licenses/by-nc-nd/4.0/), which permits non-commercial reuse, distribution, and reproduction in any medium, provided the original work is not changed in any way and is properly cited. For permission for commercial reuse, please email:[email protected]. All rights reserved.