Deposition of metal chalcogenides by metal-organic chemical vapor deposition can be achieved using various systems, including alkyl-metal-dithio or diselenocarbamates. Initial attempts to modify the behavior of such precursors by changing the nature of the carbamato ligand are reported. Among the results presented are the synthesis and characterization of the two title compounds and the single-crystal X-ray structure of one of them. For both the zinc and cadmium derivatives the films grown were of a better quality than those grown from the parent compounds or from zinc- or cadmium-diethyldithiocarbamate.