The CoFe/Cu magnetic multilayers were produced by changing CoFe ferromagnetic layers from 3nm to 10nm using electrodeposition. By now, the thinnest Cu (0.5nm) layer thicknesses were used to see whether the GMR effect in the multilayers can be obtained or not since the pinning of non-magnetic layer between the ferromagnetic layers is required. For the proper depositions, the cyclic voltammograms was used, and the current–time transients were obtained. The Cu and CoFe layers were deposited at a cathode potential of −0.3 and −1.5V with respect to saturated calomel electrode, respectively. From the XRD patterns, the multilayers were shown to be fcc crystal structures. For the magnetization measurements, saturation magnetization increases from 160 to 600kA/m from 3 to 8nm ferromagnetic layer thicknesses. And, the coercivity values increase until the 8nm of the CoFe layer thickness. It is seen that the thin Cu layer (fixed at 0.5nm) and pinholes support the random magnetization orientation and thus all multilayers exhibited the giant magnetoresistance (GMR) effect, and the highest GMR value was observed about 5.5%. And, the variation of GMR field sensitivity was calculated. The results show that the GMR and GMR sensitivity are compatible among the multilayers. The CoFe/Cu magnetic multilayers having GMR properties are used in GMR sensors and hard disk drive of the nano-technological devices.