The next generation of rotating electrical machines requires materials with an optimized combination of magnetic, electrical and mechanical properties. High-throughput experiments can accelerate the discovery of relevant materials. Past work has focused on complex multicomponent alloys in which it is difficult to pinpoint the effect of each component. On the other hand, in this work, Fe-Cu binary alloys were used as a model materials system to determine the feasibility of novel materials discovery through a rapid determination of multiple properties. The microstructures, magnetic, electrical, and mechanical properties of Fe-Cu alloys were rapidly determined. With increasing Cu content in Fe-xCu from 0 to 40 wt.%, the phases present changed from single phase BCC to a two-phase FCC+BCC microstructure. There was a decline in the saturation magnetization (Ms) from 211.3 to 118 emu/g. The hardness value increased from 166.3 HV to 238.5 HV, the coercivity (Hc) ranged from 14.6 to 45.7 Oe, and the resistivity varied between 27.3 to 43.0 μΩ.cm. The increased content of a Cu-rich phase led to a decrease in Ms and grain size, and higher Hc and hardness. Using an accelerated methodology, a significant variation in material properties was determined. Three compositions, i.e., Fe-3Cu, Fe-4Cu and Fe-10Cu, with a good balance of properties were identified for potential use in energy applications.