Cadmium bis(phenyldithiocarbamate) [Cd(PTC)] is prepared and structurally characterized. The compound crystallizes in the monoclinic space group P2/n. A one-dimensional polymeric structure is adopted in the solid state, having bridging PTC ligands and 6-coordinate pseudo-octahedral Cd atoms. The compound is soluble in DMSO, THF, and DMF and insoluble in EtOH, MeOH, CHCl, CHCl, and toluene. {CdSe[n-octylamine]} quantum belts and Cd(PTC) react to deposit epitaxial CdS shells on the nanocrystals. With an excess of Cd(PTC), the resulting thick shells contain spiny CdS nodules grown in the Stranski-Krastanov mode. Stoichiometric control affords smooth, monolayer CdS shells. A base-catalyzed reaction pathway is elucidated for the conversion of Cd(PTC) to CdS, which includes phenylisothiocyanate and aniline as intermediates, and 1,3-diphenylthiourea as a final product.