We present successful synthesis of large area atomically thin MoSe2 films by selenization of MoO3 in a vapor transport chemical vapor deposition (CVD) system. The homogeneous thin film can reach an area of 1 × 1 cm(2) consisting primarily of monolayer and bilayer MoSe2 film. Scanning transmission electron microscopy (STEM) images reveal the highly crystalline nature of the thin film and the atomic structure of grain boundaries in monolayers. Raman and photoluminescence spectroscopy confirm the high quality of as-grown MoSe2 in optics, and electronic transport measurements highlight the potential applications of the sample in nanoelectronics.