In this work, Indium Sulfide (In2S3) thin films were prepared using an economical nebulizer spray pyrolysis technique by various substrate temperatures from 250 °C to 375 °C in steps of 25 °C to evaluate their photo sensing properties. X-ray diffraction (XRD) patterns confirm the presence of In2S3 with face centered cubic structure for all substrate temperatures. The densely packed small spherical grain-sized particles were observed for In2S3 films deposited at 350 °C using Field emission scanning electron microscope (FESEM) analysis. The optical bandgap values were decreased from 3.16 eV to 2.28 eV, with increment in coating temperatures from 250 °C to 350 °C. The high intensity Photoluminescence (PL) peak is observed at 480 nm for the film coated at 350 °C is due to higher rate of electron–hole pair recombination. The photo sensing analysis revealed that the In2S3 thin films deposited at 350 °C, has the maximum responsivity (R) of 9.09 × 10−2 A W−1, detectivity (D*) of 8.25 × 1010 Jones, and external quantum efficiency (EQE) of 21.2%. Increasing the substrate temperature results in a significant enhancement of photo sensing characteristics.