Pulsed laser deposition (PLD) with different levels of laser power was first used to deposit InSfilms from homemade, high-purity InStargets. This process was followed by post-annealing in an Natmosphere to improve the films’ crystallinity and conductivity. The annealed films were verified to be stoichiometric, body-centered, tetragonal InSwith the preferred orientation (103). The bandgap of the films decreased from 2.8 to 2.2 eV with an increase in the laser power, which was believed to be the result of the grain growth caused by the higher laser power. The electrical transport property of the bottom-gate field-effect transistor revealed the n-type conduction of the annealed InSfilms, and the heterojunction p-Si/annealed InSfilm showed remarkable photovoltaic behavior upon light illumination, indicating that PLD-deposited InSfilms may have great potential as a buffer layer in thin-film solar cells. What’s more, doped InSfilms can be easily realized due to the fairly stoichiometric transfer of the PLD method.