The effects of pulse parameters on the cobalt content, surface morphologies and grain size of Zn-Co alloy deposits were studied using a pulse plating technique with a square-wave current containing reverse pulse. Average current density and reverse anodic current density amongst the variables investigated have very strong effects on the cobalt content in the Zn-Co alloy deposits. Grain size, surface appearance and internal stress in the deposit were improved significantly by introducing the reverse current. Varieties of Zn-Co alloy compositionally modulated multilayer (CMM) coatings with large differences in cobalt contents for different sublayers were electrodeposited by designing corresponding waveforms using a computer-aided pulse plater and characterized in terms of surface morphologies. Cross-sectional morphologies of the Zn-Co alloy CMM coatings, examined using field emission gun scanning electron microscopy (FEGSEM), confirmed the layered structure.