2D transition metal dichalcogenides (TMDCs) have emerged as promising candidates for post-silicon nanoelectronics owing to their unique and outstanding semiconducting properties. However, contact engineering for these materials to create high-performance devices while adapting for large-area fabrication is still in its nascent stages. In this study, graphene/Ag contacts are introduced into MoS<sub>2</sub> devices, for which a graphene film synthesized by chemical vapor deposition (CVD) is inserted between a CVD-grown MoS<sub>2</sub> film and a Ag electrode as an interfacial layer. The MoS<sub>2</sub> field-effect transistors with graphene/Ag contacts show improved electrical and photoelectrical properties, achieving a field-effect mobility of 35 cm<sup>2</sup> V<sup>-1</sup> s<sup>-1</sup> , an on/off current ratio of 4 × 10<sup>8</sup> , and a photoresponsivity of 2160 A W<sup>-1</sup> , compared to those of devices with conventional Ti/Au contacts. These improvements are attributed to the low work function of Ag and the tunability of graphene Fermi level; the n-doping of Ag in graphene decreases its Fermi level, thereby reducing the Schottky barrier height and contact resistance between the MoS<sub>2</sub> and electrodes. This demonstration of contact interface engineering with CVD-grown MoS<sub>2</sub> and graphene is a key step toward the practical application of atomically thin TMDC-based devices with low-resistance contacts for high-performance large-area electronics and optoelectronics.