High-temperature interactions between the calcium and strontium titanodisilicates were studied. It was determined that two limited series of solid solutions in the tetragonal system based on these initial compounds are formed. It was found that the changes in the physical-chemical properties of the solid solutions are discontinuous functions of solution composition. Glasses and glass ceramic materials based on the experimental system Ca2TiSi2O8– Sr2TiSi2O8 were obtained and the characteristic features of the crystallization of glass and the temperature range of the existence of the crystalline phase were determined.