Zinc and cadmium complexes of 1,1,5,5-tetraalkyl-2-4-dithiobiurets [M(N-(SCNR 2 ) 2 ) 2 ] [M = Zn, R = methy (1), ethyl (2) and M = Cd, R = methyl (4), ethyl (5)] and 1,1,5,5-tetraalkyl-2-thiobiurets [M(SON(CNR 2 ) 2 ) 2 ] [M = Zn, R = isopropyl (3) and M = Cd, R = isopropyl (6)] have been synthesized. The single crystal X-ray structures of complexes (2), ( 3), (4), and (5) were determined. Thermogravimetric analysis confirmed that all six complexes decomposed in a single step to their corresponding metal sulfides. The complexes were used as single source precursors for the deposition of zinc sulfide (ZnS), cadmium sulfide (CdS), and zinc cadmium sulfide (Zn x Cd 1-x S) thin films by aerosol assisted chemical vapor deposition (AACVD). The zinc complexes (1) and ( 3) deposited cubic ZnS films with small rods and granular crystallites at 300 and 350 °C, whereas at 400 and 450 °C hexagonal ZnS with granular crystallites were dominant. Complex (2) gave granular hexagonal ZnS films at all deposition temperatures. Cadmium complexes (4), ( 5), and (6) gave granular hexagonal CdS films at all deposition temperatures. Zn x Cd 1-x S films were deposited by varying the relative concentration of precursors ( 1) and ( 4), ( 2) and ( 5), and ( 3) and ( 6) at 400 °C. The formation of a solid solution was confirmed by UV-vis spectroscopy and powder X-ray diffraction. The morphology of the films was studied by scanning electron microscopy and atomic force microscopy. The elemental composition of films was confirmed by energy dispersive X-ray spectroscopy.