Uniform nanogranular NiFe layers with Ni contents of 65%, 80%, and 100% have been electroplated in the potentiostatic deposition mode on both planar substrates and arrays of nanowires prepared by the anodization of GaAs substrates. The fabricated planar and coaxial core-shell ferromagnetic structures have been investigated by means of scanning electron microscopy (SEM) and vibrating sample magnetometry (VSM). To determine the perspectives for applications, a comparative analysis of magnetic properties, in terms of the saturation and remanence moment, the squareness ratio, and the coercivity, was performed for structures with different Ni contents.