Light-induced photocarrier generation is an essential process in all solar cells, including organic-inorganic hybrid (CH 3 NH 3 PbI 3 ) solar cells, which exhibit a high short-circuit current density (J sc ) of approximately 20 mA/cm 2 . Although the high J sc observed in the hybrid solar cells relies on strong electron-photon interaction, the optical transitions in the perovskite material remain unclear. Here, we report artifact-free CH 3 NH 3 PbI 3 optical constants extracted from ultra-smooth perovskite layers without air exposure and assign all the optical transitions in the visible/ultraviolet region unambiguously based on density functional theory (DFT) analysis that assumes a simple pseudo-cubic crystal structure. From the self-consistent spectroscopic ellipsometry analysis of the ultra-smooth CH 3 NH 3 PbI 3 layers, we find that the absorption coefficients of CH 3 NH 3 PbI 3 (α = 3.8 × 10 4 cm −1 at 2.0 eV) are comparable to those of CuInGaSe 2 and CdTe, and high α values reported in earlier studies are overestimated seriously by extensive surface roughness of CH 3 NH 3 PbI 3 layers. The polarization-dependent DFT calculations show that CH 3 NH 3 + interacts strongly with the