Molybdenum disulfide (MoS 2 ) is a transition-metal dichalcogenide with many applications including in electronic devices and sensors. A critical issue in the development of these devices is the high resistance between the metal contact and the molybdenum disulfide layer. In this study, we employ Raman spectroscopy and X-ray photoelectron spectroscopy to investigate the modification of Au−MoS 2 contact properties using functionalized alkanethiolate self-assembled monolayers (SAMs). We demonstrate that both 2H and 1T MoS 2 strongly interact with the underlying Au substrate. The electronic properties of the interface are mediated by the dipole moment of the alkanethiolate SAM, which have a −CH 3 , −CO 2 C 6 F 5 , −OH, or −COOH terminal group. Finally, we demonstrate the site-selective deposition of 2H and 1T MoS 2 on micropatterned SAMs to form conducting−semiconducting patterned MoS 2 films.