Zinc oxysulfide nanocrystals (ZnOS NCs) were synthesized by forming ZnS phase on a ZnO matrix. ZnO nanocrystals (NCs) with a diameter of 10 nm were synthesized by forced hydrolysis in an organic solvent. As-synthesized ZnO NCs aggregated with each other due to the high surface energy. As acetic acid (AA) was added into the milky suspension of the aggregated ZnO NCs, transparent solution of well dispersed ZnO NCs formed. Finally ZnOS NCs were formed by adding thioacetic acid (TAA) to the transparent solution. The effect of recrystallization on the structural, optical and electrical properties of the ZnOS NCs were studied. The results of UV-vis absorption confirmed the band gap tunability caused by increasing the curing temperature of ZnOS thin films. This may have originated from the larger effective size due to the recrystallization of zinc sulfide (ZnS). From XRD result we identified that ZnOS thin films have a zinc blende crystal structure of ZnS without wurtzite ZnO structure. This is probably due to the small amount of ZnO phases. These assertions were verified through EDS of FE-SEM, XPS and EDS mapping of HR-TEM results; we clearly proved that ZnOS were comprised of ZnS and ZnO phases.