Crystallization of diamond in the Mg-Ge-C system has been studied at 7.5 GPa and 1800 °C with the catalyst composition ranging from pure Mg to pure Ge. It is found that with increasing Ge content of the solvent-catalyst, the degree of graphite-to-diamond conversion gradually decreases from 92 to 16%, which is a consequence of the low solubility of carbon in the germanium melt. A decrease in the Mg/Ge ratio leads to a change in the diamond growth form from cube to octahedron and a drastic increase in the number of diamond nucleation centers. The spectral properties of the crystallized diamonds are studied by photoluminescence techniques. The correlations between the Ge content of the Mg-Ge-C system and the luminescence characteristics of the diamond crystals caused by the germanium-vacancy, silicon-vacancy, and nitrogen-vacancy optical centers are established. The results obtained in this study demonstrate that by changing the catalyst composition in the Mg-Ge-C system, it is possible to control the design of the diamond crystals and synthesize isometric, pyramidal, prismatic or needle-like crystals containing Ge-V centers.