Crystalline ZnS films have been grown on a variety of substrates using chemical vapor deposition from zinc dimethyl dithiocarbarnate Zn[S2CN(CH3)(2)](2) as a single source precursor. Transmission electron microscopy and X-ray diffraction indicated that the films were composed of a uniform array of columns with cubic [1 1 1] orientation. Depth profile X-ray photoemission spectroscopy indicated that the impurity concentration remained less than 1 atomic percent (at%) in the bulk of the films. Chemical vapor deposition of zinc dimethyl dithiocarbarnate offers advantages over previous precursors to improve significantly the physico-chemical properties of ZnS films. (C) 2004 Elsevier B.V. All rights reserved.