Cu-Co materials having granular structure exhibiting good corrosion resistance as well as materials properties have been prepared from direct current (DC) and Pulse current electrodeposition (PED) technique. A comparative study of corrosion resistance as well as materials properties between the alloys (DC & PED) and multilayer (ML) were done in this paper. To understand electrolyte redox behavior, the cyclic voltammetry studies were done. The structural (X-Ray diffraction) analysis reveals that the Cu-Co alloy coating has Co0.58Cu0.42 phase and layered structures are confirmed from cross sectional scanning electron microscopy images. The chemical compositions of the deposits were observed with the help of X-Ray fluorescence technique and it reveals that the cobalt content is increased in the order of Cu-Co alloy (DC), Cu-Co alloy (PED) and Cu-Co ML. Corrosion resistance studies of the deposits were studied with Potentiodynamic polarization and electrochemical impedance spectroscopy. These studies show that the multilayer system has better corrosion resistance than the alloy system. (C) 2012 The Electrochemical Society. [DOI: 10.1149/ 2.023210jes] All rights reserved.