Electrodeposition of thin films and nanowires Ni-Fe alloys is presented. For the thin films, we have studied the impact of various electrolytic conditions (magnetic induction, pH, and substrate) on the composition and magnetic susceptibility. Whatever the electrolytic conditions, the evolution of the composition versus the polarization exhibited first a decrease of the Ni content within the deposit followed by an increase. However, at constant polarization, the obtained values were different. Concerning the evolution of the magnetic susceptibility versus the composition, it is known that it decreases with the enhancement of the Ni percentage. The reason is that the susceptibility of iron is higher than that of Ni. It can also observe a sharp rupture in the evolution of magnetic susceptibility, which appeared near the Invar composition (Ni(36)Fe(64)). Our results show that the electrolytic conditions do not affect the position of the rupture point for the thin films but modify the susceptibility values. For the nanowires, a polycarbonate membrane has been used as a template. The structural characteristics of wires were examined using X-ray diffraction. According to the composition and as described in the literature for the electrodeposited thin films, a change between the body-centered cubic structure and face-centered cubic structure was obtained for the nanowires. However, for the nanowires this modification appeared for a lower Ni content than for this in thin films. Finally, a comparison of their magnetic susceptibility with thin films exhibited a shift toward the lower Ni contents for the rupture point.