The two-dimensional layer of molybdenum disulfide (MoS2) exhibits promising prospects in the applications of optoelectronics and valleytronics. Herein, we report a successful new process for synthesizing wafer-scale MoS2 atomic layers on diverse substrates via magnetron sputtering. Spectroscopic and microscopic results reveal that these synthesized MoS2 layers are highly homogeneous and crystallized; moreover, uniform monolayers at wafer scale can be achieved. Raman and photoluminescence spectroscopy indicate comparable optical qualities of these as-grown MoS2 with other methods. The transistors composed of the MoS2 film exhibit p-type performance with an on/off current ratio of ∼10(3) and hole mobility of up to ∼12.2 cm(2) V(-1) s(-1). The strategy reported herein paves new ways towards the large scale growth of various two-dimensional semiconductors with the feasibility of controllable doping to realize desired p- or n-type devices.