The compositional effects on the physical properties including crystal structure, morphology, roughness and magnetization of Fe-Ni deposits are systematically examined in this work. All Fe-Ni deposits were fabricated by means of the pulse-reverse electroplating. The X-ray diffraction patterns show that crystalline Fe-Ni alloy and pure Fe phases coexist when the overall Fe content in the deposit is between 64 and 58 at%, while crystalline Fe-Ni alloy and pure Ni phases coexist when the overall Fe content is between 48 and 38 at%. Surface morphologies of various deposits were systematically compared by means of scanning electron microscopy (SEM) and atomic force microscopy (AFM) and found to depend on the Fe content. The roughness factor (Ra) of all deposits was also estimated from this AFM. The magnetic properties of Fe-Ni deposits were obtained from the H-M (magnetic field strength versus magnetization) diagrams. (C) 2004 Elsevier B.V. All rights reserved.