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Today, one of the most promising materials for a wide range of practical applications is lithium-containing ceramics based on Li₂TiO₃. At the same time, despite the high potential of their practical application, a number of questions remains related to the methods of their preparation, as well as the formation of a stable crystal structure and a pure-phase composition. To solve these issues, this paper proposes a method for obtaining stable Li₂TiO₃ ceramics, which is based on solid-phase synthesis combined with the high-temperature sintering of ceramics. During the studies carried out using X-ray diffraction methods, temperature dependences of phase transformations of the TiO₂/Li₂Ti₆O₁₃ → Li₂TiO₃ type were determined, according to which, at temperatures above 800 °C, the formation of a stable Li₂TiO₃ phase characterized by a high structural ordering degree of 89–91% is observed. The dependence of changes in structural, optical and ferroelectric characteristics on the conditions of synthesis and phase composition of ceramics was also determined.