In this paper, we report on the effect of sulfur additives (as FeS₂ in the Fe₉₀Ni₁₀–C system) on the growth processes, morphology, and defect-and-impurity content of diamond crystals at 6 GPa and 1400 °C. It has been established that the sulfide component plays an inhibitory role in diamond crystallization processes. As the concentration of the sulfur additive (X_S) in the system increases from 0 to 20 wt%, the degree of graphite-to-diamond transformation decreases from 100% to zero and the solubility of carbon in the melt decreases from 6.6 to 0.4 wt%. Addition of sulfur to the growth system leads to the appearance of metastable graphite and its amount increases with increasing sulfur content. It is found that the concentration of nitrogen impurities in the synthesized diamonds decreases from 50–100 ppm at X_S = 0 to 5–10 ppm at X_S = 10–15 wt%. Sulfide additives lead to the transformation of flat-faced octahedral diamond crystals to specific crystals with the elements of antiskeletal growth and fragmentation of their vertices. It is suggested that the main reason for the change in the morphology of diamond crystals is the selective adsorption of sulfide clusters on planar defects located mainly near the vertices of the octahedron. Inhibition of the propagation of growth layers on the {111} faces of diamond crystals leads to the formation of faceted macrosteps, the fragmentation of the crystal vertices and the polycentric structure of the faces.