Abstract A series of 125[NiFeCu(3nm)/Cu(1nm)] multilayers were electrodeposited on strong (110) textured Cu substrates from electrolytes containing different Fe ion concentrations under potentiostatic control. The compositional analysis by energy dispersive X-ray spectroscopy demonstrated that as the Fe ion concentration in the electrolyte is increased, the Fe content of the multilayers increased. X-ray diffraction measurements indicated that all samples exhibited a face-centred cubic structure with a strong (110) texture as their substrates. The surface images obtained by scanning electron microscopy disclosed that all films have smooth surfaces. Magnetoresistance measurements were carried out at room temperature with magnetic fields up to ±12kOe. All samples exhibited giant magnetoresistance (GMR) and the maximum GMR value of 5% was obtained in the multilayer grown from the electrolyte containing 0.0036M Fe ion concentration. The GMR magnitude changed depending on the film contents arising from the variation of the Fe ion concentration in the electrolyte. The magnetic properties studied with the vibrating sample magnetometer showed that the saturation magnetisation changed, and the coercivities decreased with varying Fe ion concentration in the electrolyte. The changes observed in the properties were ascribed to the variations observed in the film composition caused by the Fe ion concentration of the electrolyte.