The authors report on the fabrication of FeS2 (pyrite) thin films by sulfurizing Fe3S4 that were deposited by direct current magnetron sputtering at room temperature. Under the selected sputtering conditions, Fe3S4 nanocrystal films are obtained and the nanocrystals tend to locally cluster and closely pack into ricelike nanoparticles with an increase in film thickness. Meanwhile, the film tends to crack when the film thickness is increased over ∼1.3 μm. The film cracking can be effectively suppressed by an introduction of a 3-nm Cu intermediate layer prior to Fe3S4 deposition. However, an introduction of a 3-nm Al intermediate layer tends to enhance the film cracking. By post-growth thermal sulfurization of the Fe3S4 thin films in a tube-furnace, FeS2 with high phase purity, as determined by using x ray diffraction, is obtained. Optical absorption spectroscopy was employed to characterize the resultant FeS2 thin films, which revealed two absorption edges at 0.9 and 1.2 eV, respectively. These two absorption edges are assigned to the direct bandgap (0.9 eV) and the indirect allowed transitions (1.2 eV) of FeS2, respectively.