Advances made in the design and preparation of single-source precursors (SSP) involving main group elements and their use for synthesis of semiconducting materials in the form of thin films and nanoparticles are presented. A series of precursors prepared with 1,2-bis-(diethylphosphino)ethane (depe) are reported and complexes with one or two mole equivalents of the phosphine are synthesized. A series of other unsymmetrical dithio and diselenocarbamates are synthesized and used as SSPs for deposition of thin films. Bis(diethylmonothiocarbamato)cadmium is found to have some volatility despite its polymeric structure and is used to deposit films of CdS by LP-MOCVD at temperatures between 300 and 400°. Studies are concentrated towards synthesis of high-quality nanoparticles using SSPs of mixed alkyl derivatives, and these compounds are air sensitive and cannot be stored for long times.