Spherical particles of silicon dicarbodiimide (SiC2N4, see Figure) are synthesized here via the reaction of tetrachlorosilane (T) and bis (trimethylsilyl)carbodiimide (B) using pyridine as a catalyst and toluene or tetrahydrofuran as solvent. It is shown that the morphology of the thus obtained monodisperse particles strongly depends on the molar ratio of the reagents and the type and amount of solvent used.