No systematic studies have been carried out on the giant magnetoresistance (GMR) of electrodeposited (ED) Fe-Co/Cu multilayers since the elaboration of a method for the optimization of the Cu layer deposition potential. In this paper, we present results on the electrochemical optimization of the Cu layer deposition potential which was found to depend on the relative iron concentration in the bath. An X-ray diffraction study of ED Fe5Co95(1.5 nm)/Cu(d(Cu)) multilayers with d(Cu) ranging from 0.8 nm to 10 nm revealed an fcc structure. For most of the multilayers, weak superlattice satellite reflections could be identified. The room-temperature magnetoresistance was studied in detail as a function of the individual layer thicknesses. Multilayers with Cu layer thicknesses above about 1.5 nm were found to exhibit a GMR behavior with a maximum GMR of about 5% and a typical saturation field of 1 kOe. The GMR magnitude decreased with increasing Fe-content in the magnetic layer. The spacer layer thickness evolution of the MR data was established in detail after separating the ferromagnetic and superparamagnetic GMR contributions and no oscillatory GMR was found. A comparison with literature data on both physically deposited and ED Fe-Co/Cu multilayers is also made. (C) 2014 The Electrochemical Society. All rights reserved.