The large-scale synthesis of atomically thin, layered MoS2/graphene heterostructures is of great interest in optoelectronic devices because of their unique properties. Herein, we present a scalable synthesis method to prepare centimeter-scale, continuous, and uniform films of bilayer MoS2 using low-pressure chemical vapor deposition. This growth process was utilized to assemble a heterostructure by growing large-scale uniform films of bilayer MoS2 on graphene (G-MoS2/graphene). Atomic force microscopy, Raman spectra, and transmission electron microscopy characterization demonstrated that the large-scale bilayer MoS2 film on graphene exhibited good thickness uniformity and a polycrystalline nature. A centimeter-scale phototransistor prepared using the G-MoS2/graphene heterostructure exhibited a high responsivity of 32 mA/W with good cycling stability; this value is 1 order of magnitude higher than that of transferred MoS2 on graphene (2.5 mA/W). This feature results from efficient charge transfer at the interface enabled by intimate contact between the grown bilayer MoS2 (G-MoS2) and graphene. The ability to integrate multilayer materials into atomically thin heterostructures paves the way for fabricating multifunctional devices by controlling their layer structure.