The structural and optoelectronic properties of ZnO_1-xS_x alloys were investigated experimentally as well as theoretically. The ZnO_1-xS_x alloy thin films at different S concentrations (0.0 < x < 1.0) were deposited on quartz substrates by radiofrequency magnetron sputtering. The alloy composition was monitored with the help of optical emission spectroscopy. The ab initio density functional theory (DFT) based calculations were performed for the hexagonal wurtzite ZnO_1-xS_x system with the S compositions of x = 0.0, 0.0625, 0.125, 0.25, 0.5, 0.75, 0.875, 0.9375 and 1.0. The X-ray diffraction (XRD) and Raman spectroscopy measurements suggest the hexagonal wurtzite phase for the entire composition range. The films exhibit good crystalline quality with preferential growth along the c-axis. The linear change in the lattice parameter (c) was observed both from XRD analysis and DFT based calculations. The X-ray photoelectron spectroscopy confirms the anionic substitution of oxygen (O²⁻) and sulphur (S²⁻) in the hexagonal wurtzite lattice. Field emission scanning electron microscopy and atomic force microscopy were used to study the surface morphology. The optical properties were evaluated through transmittance spectroscopy and spectroscopic ellipsometry. The density of state calculations shows the forbidden region which confirms the semiconducting nature for all the alloy compositions. The energy band gap obtained from the respective Tauc's plots was found to vary from 2.9 to 3.6 eV with a bowing parameter of 3.2 eV. The same trend was observed in the calculated electronic band structures through DFT. The optical constants were evaluated from spectroscopic ellipsometry and the corresponding band gap values were compared with the values obtained from optical transmittance.