Microstructural features and surface morphologies of Ni-Fe thin films fabricated by the electrochemical deposition technique have been experimentally studied. Ni-Fe thin films have been deposited under different deposition potentials and FeSO4 concentrations. Energy dispersive X-ray measurements demonstrate that the Fe content decreases (increases) as the deposition potential (FeSO4 concentration) is enhanced. All of the produced films exhibit an anomalous codeposition behavior. The effects of deposition potential and FeSO4 concentrations on the degree of anomalous codeposition have been also characterized. X-ray diffraction studies reveal that the films have face-centered cubic crystallographic structures with  preferred crystallographic orientation regardless of the applied deposition conditions. However, the crystallization and the crystallite size of the films are affected by changing of the FeSO4 concentration and the deposition potential. The results of scanning electron microscopy analyses verify that the surface structure of the film electroplated from the electrolyte with higher FeSO4 concentration under higher deposition potential exhibits a more homogeneous and dense structure with smaller grain sizes.