CaS:Eu2+ red-emitting phosphors particles, were prepared by the precipitation method, followed by sintering in the atmosphere over the mixture of sulfur powder, Na2CO3, and carbon-containing compounds such as tartaric acid, citric avid, glucose, and cane sugar. The structure, morphology and photoluminescence performance of the as-prepared samples were investigated by X-ray powder diffraction (XRD), transmission electron microscopy (TEM), and photoluminescence spectrum (PL), respectively. The influences of carbon-containing additives on its crystallization behavior, morphology, and enhancement in luminescence of CaS:Eu2+ particles were studied. CaS:Eu2+ particles without additive show inhomogeneous, rough and aggregation with the size of 75-125 nm, but the spherical particles with mean size of about 110 nm were obtained by adding carbon-containing compounds. Compared with phosphor without additive, the addition of carbon-containing materials induced a remarkable increase of PL, in the order of cane sugar, glucose, citric acid, and tartaric acid. This enhancement is duo to the improvement of crystallinity, particle morphology and size distribution of the samples by adding carbon-containing additive.