Molybdenum disulfide (MoS2) films, which are only a single atomic layer thick, have been synthesized by chemical vapor deposition (CVD) and have gained significant attention due to their band-gap semiconducting properties. However, in order for them to be useful for the fabrication of practical devices, patterning processes that can be used to form specific MoS2 structures must be integrated with the existing synthetic approaches. Here, we report a method for the synthesis of centimeter-scale, high-quality single-layer MoS2 that can be directly patterned during CVD, so that postpatterning processes can be avoided and device fabrication can be streamlined. Utilizing X-ray photoelectron spectroscopic imaging, we characterize the chemical states of these CVD-synthesized single-layer MoS2 films and demonstrate that the triangular-shaped MoS2 are single-crystalline single-domain monolayers. We also demonstrate the use of these high-quality and directly patterned MoS2 films in electronic device applications by fabricating and characterizing field effect transistors.