The application of a pure FeCo film directly to devices is limited by the intrinsic properties of a homogeneous monolayer of the alloy, despite it having the highest saturation magnetization. A feasible methodology based on alternating current‐density electrodeposition to tune the microwave properties of FeCo films through diverse atom‐stacking arrangements is reported. The properties range from a large relative resonance permeability (up to 728 in the real part) to ultrahigh resonant frequency (up to 5.2 GHz), and extremely wide frequency dispersion (1.5–6.0 GHz); these are not observed in other materials or as a result of conventional doping methods. They are attained using different single‐layer, semi‐multilayer, and multilayer FeCo nanofilms, fabricated by diverse stacking arrangements of Fe and Co atoms during deposition in a single bath. This technique firstly exemplifies the significant effect of atom arrangement on magnetic inhomogeneity, nanoscale morphology, composition, crystal texture, stress, and damping, which in turn largely alters both the static and dynamic magnetic properties of the ferromagnetic film. These thin FeCo films might be used directly in various devices operating in the gigahertz frequency range.