Ferromagnetic nanofilms with high saturation magnetization (Ms), particularly FeCo alloys with the highest Ms value (theoretically 2.45T), are promising candidates for emerging compact high-performance magnetoelectronic, microwave, and spintronic devices. Thin films with diverse and specific dynamic microwave properties are essential components for these different applications. For example, a high-frequency mobile phone requires a ferromagnetic element of high resonant frequency (fr) ; [4] a thin single-band microwave absorber requires ferromagnetic films with large resonance-type permeability (m), whereas a broadband absorber requires films with wide frequency dispersion or large relaxation-type m. The demand for a wide range of functions poses challenges for both scientific understanding and fabrication of these thin films, in particular, for applications in gigahertz (GHz) range. Hence despite being one of the earliest themes in magnetism, the topic of ferromagnetic thin films for high-frequency applications still generates much interest from scientists and engineers. Although the influence of the composition of materials on static or dynamic magnetic properties is well studied and described mathematically, for example, by Snoek’s law and constant (S), 3, 15] most formulae are insensitive to the crystal structure or nanostructure of thin ferromagnetic films. The understanding of the influence of an altered structure on the static and dynamic magnetic properties is still limited. A notable example is the preparation of appropriate nanostructure or crystal texture of soft ferromagnetic thin films with high Ms, such as FeCo, for achieving low coercivity (Hc 50 Oe), as well as ultrahigh fr ( 5 GHz) or wide frequency dispersion ( 3 GHz) by simple diverse atom arrangements without the addition of other materials. 17] Due to the inherent limitations of pure homogeneous ferromagnetic single-layer films (e.g. undesirable magnetic softness, anisotropy, or crystallinity of FeCo films), and a lack of evidence on the relationship between the nanostructure or crystal texture and dynamic microwave properties, doping or insertion of nonmagnetic materials is often used to address the stringent requirements of functional devices. This has be achieved by adding AlOx to a FeCo(HfO) film to attain a high fr ( 3 GHz), utilizing FeCo–MnIr exchange-coupled multilayers for wideband microwave noise filtering, or by doping Zr or B into a ferromagnetic film to adjust the m type. However, there are two critical challenges associated with these methods. The foreign elements decrease the Ms of the ferromagnetic film and subsequently deteriorate the device efficiency or performance. Moreover, most of the modifications are tailored 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.