Amorphous metal alloys play an important role in the electrical industry. Studies show the presence of an insignificant proportion of crystals in alloys that are amorphous from the point of view of X-ray diffraction analysis. The crystals significantly affect the mechanical and magnetic properties of amorphous alloys. Therefore, within this work, a comprehensive approach has been developed to determine the degree of crystallinity of amorphous alloys based on theoretical and experimental methods. The study is based on the mathematical model of supercooled melt crystallization previously developed by the authors, which takes into account the patterns of crystal formation and their diffusion and diffusionless growth, taking into account the mutual influence of growing crystals on each other. The mathematical model also takes into account the melt cooling mode when producing amorphous ribbons by cooling the melt on a rotating copper drum. The calculation results have been verified by experiments based on the new technique developed by the authors for calorimetric studies of amorphous ribbons. The developed methodology allows us to determine not only the average fraction of the crystals in a ribbon, but also the patterns of crystal distribution along its thickness as well as the patterns of changes in the proportion of the crystals in ribbons depending on the melt cooling mode.