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Cadmium sulfide (CdS) nanoparticles have been synthesized from CdX2 (X = Cl–, I–) complexes of 4-chlorobenzaldehyde and benzophenone thiosemicarbazone. The complexes have been studied by thermogravimetric analysis (TGA), elemental analysis, FT-IR, and NMR spectroscopy. The solvothermal decomposition of the complexes has afforded oleylamine-capped CdS nanoparticles with a wurtzite hexagonal phase. The transmission electron microscopy (TEM) studies show different morphologies which are influenced by reaction temperature and the nature of the ligands on the precursor complexes. Particles in the form of irregular cubes, elongated cubes and nanodendrites have been observed. The UV-Vis spectroscopy measurements show temperature and nature of complex-dependant optical properties. Blue-shifted band gap energies have been observed at lower reaction temperatures.