This paper describes an improved strategy for controlling the adhesion force using both the antiadhesion and adhesion layers for a successful large-area transfer process. An MPTMS (3-mercaptopropyltrimethoxysilane) monolayer as an adhesion layer for Au/Pd thin films was deposited on Si substrates by vapor self assembly monolayer (VSAM) method. Contact angle, surface energy, film thickness, friction force, and roughness were considered for finding the optimized conditions. The sputtered Au/Pd (~17 nm) layer on the PDMS stamp without the anti-adhesion layer showed poor transfer results due to the high adhesion between sputtered Au/Pd and PDMS. In order to reduce the adhesion between Au/Pd and PDMS, an anti-adhesion monolayer was coated on the PDMS stamp using FOTS (perfluorooctyltrichlorosilane) after O2 plasma treatment. The transfer process with the anti-adhesion layer gave good transfer results over a large area (20 mm × 20 mm) without pattern loss or distortion. To investigate the applied pressure effect, the PDMS stamp was sandwiched after 90˚ rotation on the MPTMS-coated patterned Si substrate with 1-μm depth. The sputtered Au/Pd was transferred onto the contact area, making square metal patterns on the top of the patterned Si structures. Applying low pressure helped to remove voids and to make conformal contact; however, high pressure yielded irregular transfer results due to PDMS stamp deformation. One of key parameters to success of this transfer process is the controllability of the adhesion force between the stamp and the target substrate. This technique offers high reliability during the transfer process, which suggests a potential building method for future functional structures.