We report on the improvement of the electronic characteristics of monolayer graphene field-effect transistors (FETs) by an interacting capping layer of a suitable fluoropolymer. Capping of monolayer graphene FETs with CYTOP improved the on-off current ratio from 5 to 10 as well as increased the field-effect mobility by as much as a factor of 2 compared to plain graphene FETs. Favorable shifts in the Dirac voltage toward zero with shift magnitudes in excess of 60 V are observed. The residual carrier concentration is reduced to ~2.8 × 10(11) cm(-2). Removal of the fluoropolymer from graphene FETs results in a return to the initial electronic properties before depositing CYTOP. This suggests that weak, reversible electronic perturbation of graphene by the fluoropolymer favorably tune the electrical characteristics of graphene, and we hypothesize that the origin of this improvement is in the strongly polar nature of the C-F chemical bonds that self-organize upon heat treatment. We demonstrate a general method to favorably restore or transform the electrical characteristics of graphene FETs, which will open up new applications.