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In this work, iron sulfide thin films were prepared by simple and low-cost chemical spray-pyrolysis method (CSP) using tilt deposition with a spraying angle of 45° and substrates temperature (200°C, 350°C). The precursors were iron nitrate (Fe (NO3)3.9H2O) and thiourea. The study shows the feasibility of using iron sulfide as a counter electrode in Dye-sensitized solar cells. It was found that the iron sulfide thin films with an amorphous structure gave the highest absorption coefficient (1.8×105cm−1) and highest conversion efficiency (1.8%) in DSSCs. This work also investigates the optimum conditions of substrate temperature, annealing temperatures, and the presence of sulfur powder and argon gas to obtain polycrystalline pyrite thin films with optimum energy gap and high absorption coefficient. [ABSTRACT FROM AUTHOR]