In the present investigation we have galvanostatically synthesized nanocrystalline Fe-Ni alloys on copper substrate. The effect of current density (c.d.) on composition, surface morphology and phase structure were studied for explaining the magnetic and electrochemical properties of the nanocrystalline alloy. The bath found to exhibit the preferential deposition of less noble Fe than Ni, and at no conditions of c.d., the deposition has changed from anomalous to normal type. Surface morphology and structural characteristics of the deposits were examined using scanning electron microscopy (SEM) and X-ray diffraction (XRD) analysis. As composition of the alloy varied, consequent to the current density a change of body centered cubic structure (bcc) to face centered cubic structure (fcc) was observed for nanocrystalline materials. Finally, the conditions responsible for peak magnetic property and corrosion resistance were optimized. Factors responsible for improved functional properties were explained in terms of surface morphology and crystalline grain size of the coatings. (C) 2012 Elsevier B. V. All rights reserved.