We report optical properties of iron pyrite (FeS2) determined from ex situ spectroscopic ellipsometry measurements made on both a commercially available bulk single crystal and nanocrystalline thin film over a spectral range of 0.735-5.887 eV. The complex dielectric function, ε (E) = ε 1 (E) + iε 2 (E), spectra have been determined by fitting a layered parametric model to the ellipsometric measurements. Spectra in ε are modeled using a Kramers-Kronig consistent critical point parabolic band model involving seven critical points for the bulk single crystal and four critical points for the nanocrystalline film. Absorption coefficient spectra for both types of samples are also determined from ε. Critical point features in the nanocrystalline films are broader, have lower amplitude and lower energy critical points detected having a small blue shift when compared to the single crystal sample.