M. Tech. (Department of Chemistry, Faculty of Applied and Computer Science), Vaal University of Technology / Cadmium and cobalt complexes of urea and thiourea were synthesized using ethanol as a solvent. All complexes were refluxed at 70 - 80 °C, left to cool at room temperature, washed with methanol and acetone to remove impurities and dried at an open environment. The characterization of complexes was done using FTIR spectroscopy, elemental analysis and TGA. The complexes were found to coordination with the ligands through sulphur and oxygen atoms to the metal, instead of nitrogen. These were as results of wavelength shifting from high to low frequency from spectra of the complexes as compare to their free ligands. These observations make these complexes good candidates for the possible use in synthesis of metal sulphides or oxides nanoparticles. Thermogravimetric analyses of all the complexes were conducted to check the stability of use as precursors for nanoparticles at low and high temperature. A number of thiourea and urea complexes with cadmium and cobalt have been prepared and used in the preparation of metal sulphides/oxides nanoparticles. Complexes start to decompose at low temperature about 100°C and the last decomposition step was at about 800-900°C, which is convenient to thermal decomposition of precursors in the high boiling solvents or capping agent to prepare surface capped metal sulphides/oxides nanoparticles. The complexes were easy to synthesize, low cost and stable in air and were obtained in reasonable yields. All the complexes reported in this study have been used as single source molecular precursor in the preparation of cadmium oxide, cadmium sulphide, cobalt oxide, cobalt sulphide nanoparticles (normal) and as mixture of any two complexes to form core-shells nanoparticles. Quality nanoparticles synthesis requires three components: precursors, organic surfactants and solvents. The synthesis of the nanoparticles can be thought of as a nucleation event, followed by a subsequent growth period. Both the nucleation and growth rates were found to be dependent upon factors such as temperature, growth time, and precursor concentration. For a continuous flow system the residence time (at nucleation and growth conditions) was also found to be important. In order to separate the nucleation and growth events, injection techniques were employed to achieve rapid nucleation of nanoparticles with final size dictated by the growth temperature and/or residence time through the growth zone of the reaction system. Good crystalline normal nanoparticles were obtained from thermolysis of the precursors in hexadecylamine (HDA) as the capping agent at fixed concentrations, temperature and time. All nanoparticles showed a blue-shift in band edges with good photoluminescence behaviour which is red-shifted from their respective band edges and XRD patterns, the crystal structure are in hexagonal phase. The particles showed rods, spheres and hexagonal shapes. Nucleation and growth mechanism brings new avenue in nanostructures called core-shells, which have been reported to have improved luminescence, quantum yields, decreased fluorescence lifetimes, and benefits related to the tailoring of the relative band-gap positions between the two materials. In this study cadmium and cobalt complexes of urea and thiourea were separately dispersed in TOP and injected separately (allowing nucleation/core to occur, followed by the shell) in hot HDA at 180ºC for 1hour to yield core-shell nanoparticles. Parameters, such as concentration, temperature and capping molecule as factor affecting nucleation and growth of the core-shells were monitored. The core-shell nanoparticles were characterized by UV/Vis spectroscopy, XRD and TEM. We observed spherical, tripod, bipods, hexagonal and irregular shaped nanoparticle as the concentration of the precursors was increasing, however we were able to form core-shells nanoparticles in one set of experiment 1:3 CdS-CdO, which are assumed to be a reverse type I coreshells nanoparticles. Exciton absorption peaks at higher energy than the fundamental absorption edge of bulk indicate quantum confinement effect in nanoparticles as a consequence of their small size. XRD patterns, crystals range from hexagonal, cubic and mixture of hexagonal and orthorhombic. A low temperature studies were also conducted a mixture of hexagonal and sphererical shapes with sheets like onion morphology were observed. / NRF HUB & SPOKES (VUT)