Ultrasoft magnetic materials, such as amorphous, nanocrystalline, and polycrystalline alloys, have been successfully used for power electronic applications during recent years. However, enhancements are needed for the integration of power electronic features, which involves high power densities and operating frequencies up to a few megahertz. Complex permeability spectra, which are used to describe material behavior in these applications, depend mainly on domain-wall motions and coherent magnetization rotation mechanisms. In this paper, we present a model describing these mechanisms, in terms of magnetic anisotropies and domain structure of the material. To validate the model, we measured permeability spectra of polycrystalline Ni-Fe alloys under mechanical stress using a specific setup. These measurements are suitable for comparing the physical model according to different magnetoelastic anisotropies. Results are useful for correlating high-frequency magnetic behavior and the annealing process of materials.