In this report we describe some experimental results concerning the preparation by electrodeposition and characterization of Co/Zn multilayer films, a system of special significance because Co and Zn are immiscible in a large range of compositions, permitting an easier adaptation of the sharp interfaces and the magnetic interactions between layers, with a view to obtain technological applications in nano-electronics. We established the working parameters for electrodeposition of multilayer films based on Co and Zn nanoscale layers, using a dual-bath potentiostatic electrodeposition method. The effect of the first electrodepositecl layer growth process on the structure and magnetic properties of the multilayer were studied by using two series of multilayers of varying periods, starting with Co or Zn layers, respectively (with the same total thickness of Co layers, namely 50 layers of 5 nm thick, but various Zn layer thickness). These properties were also studied as a function of the Zn layer thicknesses (varying between 0.1 nm and 5.9 nm), for the two series of films. The magnetoresistance (in the current in plane configuration with dc magnetic field applied in the film plane), varied with Zn layer thickness, exhibiting a giant magnetoresistance contribution of about 30% in the case of [Co (5 nm)/Zn (2.7 nm)](50) films. (C) 2011 Elsevier B.V. All rights reserved.