The effects of applied voltage on the magnetic and mechanical properties of polyol electrodeposited NiCo films were studied and reported. Both electroless and electrolytic processes competed with each other during deposition. There existed a clear influence of voltage on the composition and magnetic properties of deposited films. However, a simple, systematic correlation of these properties with the structure, composition and microstructure could not be made. This lack of correlation was attributed to the complex variation of deposition chemistry with deposition time and voltage. It is conceivable that thick films deposited using long reaction time may have through-thickness inhomogeneity, thus obscuring the correlation of properties with the volume-averaged film characteristics.