This chapter provides a brief description of mechanosynthesis and its applications in the preparation of perovskite-type materials. A historical development of mechanochemistry is reviewed, followed by the basic information on the mechanosynthesis process, microstructural development, and chemical reactions occurring under mechanical actions. The milling devices, usually used for perovskite preparation, were described. A particular emphasis is made on the evolution of the physicochemical properties of perovskites, synthesized by high-energy ball milling, and their beneficial effects for different applications. The advantages and drawbacks of the mechanosynthesis in preparation of perovskites are discussed.