Monodisperse ZnS colloidal particles with precisely specified diameters over a broad size range were synthesized by controlled aggregation. Sub-10nm ZnS seed crystals were first nucleated at ambient temperature and then grown at an elevated temperature, which produced large polydisperse colloidal particles. Subsequent rapid thermal quenching and heating processes induced a number of secondary nucleations in addition to growing the large polydisperse microparticles which were finally removed by centrifugation and discarded at the completion of the reaction. The secondary nuclei were then aggregated further at elevated temperatures, resulting in colloidal particles which exhibited a nearly monodisperse size distribution. Particle diameters were controlled over a wide size range from 50 nm to 1 μm. Mie simulations of the experiment extinction spectra determined that the volume fraction of the ZnS is 0.66 in an aggregated colloidal particle and the colloidal particle effective refractive index is approximately 2.0 at 590 nm in water. The surface of the colloidal particles was subsequently coated with silica to produce ZnS@silica core-shell particles.