In recent years, ferrite nanoparticles have been considered as promising functional materials for high-density data storage devices [1][2][3][4]. Such materials can be prepared as thin films, dispersed powders, and composites [1,4]. Manganese ferrite nanoparticles were crystallized from melts of potassium aluminum borate glass ( K 2 O-Al 2 O 3 -B 2 O 3 ) with additions of iron(III) and manganese(II) oxides [5][6][7][8][9]. The particles were detected by X-ray diffraction and transmission electron microscopy [6][7][8]. Their size ranged from 5 to 50 nm depending on the synthesis conditions. The resulting glasses were transparent and exhibited the properties of magnetically ordered systems with high magnetization and Faraday effect values, including the remanent value, in relatively weak magnetic fields [8]. Efforts have been made to estimate the degree of clustering of magnetic ions by measuring the magnetic and optical properties of glasses [10][11][12]. However, the character of the change in these properties depended not only on the particle size. The measured integral properties of glasses are not unambiguously interpretable without knowledge of the actual composition and structure of ferrite nanoparticles, which determine the distribution of Mn and Fe cations over magnetic sublattices.In this work, the actual composition and structure of ferrite nanoparticles dispersed in glass were determined for the first time by using the differential dissolution (DD) method and high-resolution transmission electron microscopy (HRTEM). This task was challenging for small particles and their low content and nonuniform distribution in the glass matrix. In addition, determining the components of the glass itself in the ferrite against the background of the glass matrix is conjectural, although such a determination is mandatory for interpretation of the magnetic and optical properties of glass.Glass samples with different oxide contents were prepared at the Vavilov State Optical Institute by the procedure described in [9]. A series of glasses of different composition was studied. In this work, we discussed the results of studying glasses with an overall content of Fe and Mn oxides of 3 wt % and the atomic ratio Mn/Fe = 0.86; i.e., the manganese content of the glass was nearly twofold higher than that required by the ferrite stoichiometry. The magnetic and magnetooptical characteristics of this sample ( M H = 10 kOe = 0.49 emu/g, M H = 2.0 kOe = 0.39 emu/g, α H = 2.0 kOe = 7.35 deg/cm, α / M = 18.85), as well as of the other samples synthesized by this technique, deviated noticeably from the analogous characteristics of massive manganese ferrite with regard to the content of the ferrite phase in glass. It was necessary to elucidate the nature of these deviations with the aim of improving the magnetic and magneto-optical properties of glasses.Stoichiometry of manganese ferrite nanoparticles. The compositions of the matrix and nanoparticles were determined by the differential dissolution method [13,14]. The analysis was carried o...