The phase-controlled synthesis of ZnS nanocrystallites from an air-stable single-source molecular precursor (zinc diethyldithiocarbamate: Zn-(DDTC)(2)) has been achieved by two facile steps: firstly, the Zn-(DDTC)(2) was prepared directly via the precipitation reaction of zinc acetate and sodium diethyldithiocarbamate in distilled water under ambient condition; secondly, pure Cubic and hexagonal phases of ZnS nanocrystallites could be obtained just by low-temperature (150-200 degrees C) solvothermal decomposition of the Zn-(DDTC)2 in distilled water and ethanol, respectively. The as-obtained products were characterized by powder X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), transmission electron microscopy (TEM) and UV-vis absorption spectra. (c) 2005 Elsevier B.V. All rights reserved.