We report a new route to synthesize high quality zinc blende CdS and ZnS nanocrystals in noncoordinating solvent 1-octadecene, using dodecanethiol (DDT) molecules as both the sulfur source and surface capping ligands. Different reaction temperatures and Cd(Zn)/DDT molar ratios were tested to optimize the synthesis conditions. Absorption photoluminescence (PL) spectroscopy, Fourier transform infrared (FTIR) spectroscopy, X-ray diffraction (XRD) pattern, and transmission electron microscopy (TEM) were used to characterize assynthesized nanocrystals. The narrow half width at the half-maximum on the long wavelength side of the firstexcitonic absorption peak and TEM images demonstrated nearly monodisperse size distributions of asprepared CdS, ZnS, and CdS/ZnS core/shell nanocrystals. Only trap emissions of the nanocrystals were detected when the amount of DDT was excessive, this came from the strong quenching effect of thiol groups on the nanocrystal surfaces. After overcoating with ZnS shells, band-gap emissions of CdS nanocrystals were partially recovered.