Future electronics technology is expected to develop from rigid to flexible devices. This process requires breakthroughs in material properties, especially flexibility, in combination with desirable electrical insulating, semiconducting, or metallic properties. Graphene, being one of the recently developed two-dimensional (2D) materials, presents great promise as an active layer in a wide spectrum of electronics devices and, first of all, in field-effect transistors (FET). The development of optimized dielectrics for the graphene active layer is critical for graphene applications. The carrier transport in graphene films takes place at interfaces with dielectric or semiconductor substrates; therefore, the quality of such interface and the interaction of graphene films with nearby dielectric layers (charge carrier scattering) determine the device performance. Generally, the development of dielectric materials aiming at high performance device operation, proper mechanical properties, and low-temperature fabrication is not progressing well since the graphene thin film is very sensitive to surface conditions of dielectric layers. Solving the problem with dielectric layers in the case of nonorganic printed and flexible electronics is especially acute. As it is demonstrated in the present chapter, dielectric layers fabricated from fluorinated graphene suspension or in its combination with graphene oxide are the most promising for graphene-based flexible, printed, and transparent electronics.