Physicochemical processes of the fluoride processing of kyanite concentrates under the influence of additional components are studied theoretically and experimentally in the range of temperatures of 20–550°C and curing times of 0.12–4.5 h. The optimal conditions of feed stock sintering with ammonium bifluoride, sublimation of ammonium hexafluorosilicate, formation of aluminum fluoride and alumina, and synthesis of amorphous silica nanoparticles are found. Thermodynamic and kinetic parameters of chemical reactions are calculated. The studies are used as a basis for the development of the fluoride method of alumina generation from kyanite concentrates with the complex recovery of other useful components.