Laser irradiation for tuning the optoelectronic parameters of semiconducting thin films is widely applicable and has many benefits. The aim of the study is 532 nm laser irradiation of Te/In2Se3 film at different laser exposure time scales. The bilayer structure and its conversion to a single layer with laser annealing were confirmed from cross-sectional scanning electron microscopy. At the same time, the element's appearance was found in the EDX analysis. FESEM probed the corresponding surface structure change. XRD and Raman's spectroscopy analyzed the increase in crystallinity with laser irradiation by mixing Te into the In2Se3 layer and related microstructural changes. The shift in Raman peak with lasing time signifies the effect of time of exposure. There is a systematic decrement in the transmittance of the films. Also, the absorption edge shift resulted in the decrement in bandgap with laser irradiation. The static refractive index and optical density increased as well. The skin depth was decreased with a minimal change in the optical electronegativity. The nonlinear refractive index increased from 1.638 × 10–9 esu to 1.773 × 10–9 esu by 60 min laser irradiation. Similarly, there was an increment in 3rd-order nonlinear susceptibility from 1.58 × 10–10 esu to 1.73 × 10–10 esu. The surface wettability test confirmed the hydrophilic nature of the samples with decreasing hydrophilicity by laser irradiation. The tuning in different properties of the Te/In2Se3 film by laser irradiation is suitable for various optoelectronic applications.