Calcium phosphates have been used extensively as biomaterials for bone tissue repair and regeneration since they are found in biological organisms, and are the inorganic components of human bones and teeth. Nowadays, there is particular interest in nano-sized inorganic crystals for use as calcium phosphate bone substitutes, especially tricalcium phosphate and hydroxyapatite. The emphasis of the Doctoral Thesis was on the understanding of the current development of the most widely used calcium phosphates that could contribute to applications in calcium phosphate bone cements and biocomposite coatings. The literature review provides an overview of calcium phosphates for biomedical applications, their physical–chemical properties and synthesis methods concerning the period from 1970 to 2015. The efficient synthesis technology for fast production of nano-sized calcium phosphates has been developed, and the potential applications of these materials have been investigated. The results of the Doctoral Thesis demonstrate the possible further applications as biomedical materials with the potential of the clinical efficiency. The Doctoral Thesis can be viewed as the phase of basic principles continuing the technological research to develop a new approach to the pilot production of nano-sized calcium phosphates, α-tricalcium phosphate, β-tricalcium phosphate and hydroxyapatite. In addition, it is planned to continue investigating their further applications as biomedical materials. The Doctoral Thesis has been written in English and consists of 120 pages. The Doctoral Thesis contains 43 figures, 18 tables, 35 equations, 17 appendices and 254 references. The Doctoral Thesis is organized as a series of relatively independent chapters: 1) Preparation and application of nano-sized α-tricalcium phosphate; 2) Preparation and application of nano-sized hydroxyapatite and β-tricalcium phosphate; 3) Transforming laboratory studies into technology concept.