Different PbX2 (X = AcO, Cl, Br, I) metal salts were complexed to cinnamaldehyde thiosemicarbazone ligand. The resulting complexes were characterised using Fourier Transform Infrared spectroscopy, 1H and 13C {1H} Nuclear Magnetic Resonance spectroscopy, elemental analysis and thermogravimetric analysis techniques. They were then used as single source precursors for the preparation of lead sulfide (PbS) nanoparticles using the colloidal thermolysis route where oleylamine is used as the passivating agent. Each SSP is thermolysed at reaction temperatures of 190, 230 and 270 °C. Predominantly cubic-shaped PbS nanoparticles were obtained, with an exception of the truncated nanocubes obtained from thermolysis of the SSP prepared from lead bromide. Varying particle sizes are obtained when the halogen is varied, ranging from ca. 50 to 400 nm. The optical absorbance of the PbS nanoparticles in the UV-Vis- NIR range was found to be blue-shifted when compared to bulk PbS.National Research Foundation (NRF), South Africa (NRF Grant Number 64820), the India–Brazil–South Africa (IBSA) program, Royal Society Department For International Development (RS-DFID) program and the Department of Science and Technology (DST)-PURSE, India,