The synthesis of large-area graphene by the chemical vapor deposition (CVD) method is a mature technology; however, a transfer procedure is required to integrate CVD-grown graphene into a functional device. The reported methods for transferring graphene films cause different degrees of defects (cracking, rupture) and ion/polymer residues, which deteriorate or alter the electrical properties of as-grown graphene. Developing a reliable and fast transfer method that can maintain high-quality graphene remains a challenge. In this work, we employed UV light release tape (UV-RT) as the support layer to replace the frequently used thermal release tape (TRT) in a typical roll-to-roll dry transfer process. In this process, we used an easier-to-remove polymer as an adhesion layer to greatly reduce the strain and defects that occur during the transfer process. The cleanliness of graphene transferred by this method is above 99%, and the carrier mobility is 1.6 and 1.1 times higher than that obtained with conventional wet transfer and TRT transfer methods, respectively. UV illumination leads to facile and uniform release of the graphene film onto the target substrate, achieving one-step and selective patterning of graphene (feature size of <100 μm). The UV-assisted decomposition of the polymer molecular structure into small molecules enables a residue-free and ultraclean graphene surface. This proposed transfer method enables facile patterning of graphene and 2D films while maintaining high quality, which paves the way for versatile functional graphene applications.