The two-dimensional (2D) layered molybdenum disulfide (MoS2) material represents a nominee potent for optoelectronic devices application. In this research work, the experimental characterizations of 2D- MoS2 thin films are reported in terms of various microscopic and spectroscopic techniques. The synthesized MoS2 thin films are grown by employing the pulsed laser deposition (PLD) procedure on SiO2/Si substrates. In order to monitor the deposition rates of ablated films, the buffer argon-gas pressures are varied during the pulsed laser deposition at substrate temperature of 700 °C. The field emission scanning electron microscopy and atomic force microscopy analyzes revealed a change in the surface morphology of MoS2 films when the buffer Ar-gas pressure is varied between 0 and 100 mTorr. For all samples, a 2H-phase is revealed from X-ray diffraction patterns, indicating a reflection (2θ) around 14.85°. By varying the deposition pressure of laser-ablated MoS2 films, the X-ray photoelectron spectroscopy divulged the chemical compositional elements and valence states of Mo and S on the surface of MS2 films with low density of defects. Analysis of the photoluminescence spectroscopy illustrated emission bands spanning from the visible (Vis) to near-infrared (NIR) regimes in the deposition pressures range ~ 0–100 mTorr. This is mainly owing to the change in the recombination of electron–hole pairs and charge transfer between the deposited MoS2 films and SiO2 substrate surface under various buffer gas pressures. Additionally, first-principles electronic structure calculations are performed to qualitatively examine the effect of native point-defect species (sulfur-monovacancy and sulfur-divacancy defects) on the electronic structure and optical properties of 2D- MoS2 sheets. It is unveiled that the variation of compositional sulfur-vacancy defect in MoS2 monolayer creates an in–gap defect levels above the valence states, leading to an acceptor character. Importantly, the enhancement in the optical absorption spectra divulged a shift in the optical gap from Vis-NIR window with the increase of sulfur vacancy contents in MoS2 single-layer. The identification of intrinsic point defects may be beneficial for photovoltaic energy conversion at higher wavelengths by designing next generation 2D-semiconductors, which could be of vital significance for growing 2D layers and multilayers into practical technologies.