This thesis work elaborates a facile technique for fabrication of functionally graded all graphene films using a one-step film coating process. The film coating consists of interfacial reduction and self-assembly of a graphene oxide (GO) precursor on an active metal substrate. Processing parameters such as the underlying substrate metal and the film drying environment are controlled in order to tailor the internal architecture of the films and to achieve functionally graded structure during the reduction of GO. The self-assembly and functional grading of the films, where one side is electrically conductive reduced GO (rGO) and the opposite side is insulating GO, was confirmed by SEM, Raman, XRD, FTIR, and XPS characterization studies. All graphene based free standing films with selectively reduced GO were used in transient electronics application as flexible circuitry and RFID tag antenna where their decommissioning was easily achieved by capitalizing on GO’s ability to readily dissociate and create a stable suspension in water. Furthermore, the functionally graded structure was found to exhibit differential swelling behavior and its potential applications in graphene-based actuators were outlined.