Bis-3-methylpyridine and bis-4-methylpyridine complexes of cadmium(II) ethylxanthate have been characterized by elemental analysis, NMR spectroscopy, and thermogravimetric analysis. The single crystal X-ray structures of both methylpyridine derivatives have also been determined and shown to display a cis, cis, cis-configuration of the N-And S-donor ligands. The compounds have been utilized as single source precursors to deposit CdS films on silica-coated glass substrates at 220 and 350 °C by aerosol-Assisted chemical vapor deposition. The surface morphology of the films has been examined by scanning electron microscopy analysis and the crystalline phases were studied by powder X-ray diffraction. The films deposited from the 3-methylpyridine adduct comprised more densely packed and more highly crystalline hexagonal CdS than those provided by either of the other two precursors. The crystallite sizes were found to be g = 2.25-2.40 eV) consistent with bulk CdS.