Ni-Cu/Cu multilayers have been, grown from a single electrolyte under potentiostatic conditions at different electrolyte pH values. The current-time transients recorded during deposition indicated different growth modes of the Ni-Cu layers. Structural characterisation by X-ray diffraction revealed that the multilayers have the same crystal structure and texture as their ( 1 0 0) textured polycrystalline Cu substrate. Scanning electron microscopy showed that the films grown at low pH (2.2) have smoother surfaces than those grown at high pH (3.0). Energy dispersive X-ray analysis revealed that the magnetic layers of the multilayers electrodeposited at high pH contain much more Cu compared to those deposited at low pH. Anisotropic magnetoresistance was found for nominal Cu layer thicknesses below 0.6 nm, and giant magnetoresistance (GMR) above 0.6 nm. The shape of the magnetoresistance curves for GMR multilayers indicated the predominance of a superparamagnetic contribution, possibly due to the discontinuous nature of the magnetic layer. For multilayers with the same bilayer and total thicknesses, the GMR magnitude decreased as the electrolyte pH increased. Besides possible structural differences, this may have come from a strong increase in the Cu content of the magnetic layers since this causes a nearly complete loss of ferromagnetism at room temperature.