Fluorine and oxygen co-doped graphene with controllable element coverage was effectively synthesized through simultaneously fluorinating and reducing graphene oxide by pyrolysis of fluorinated graphite. Morphology investigation indicates that the doped graphene is of few-layered thickness, and the prepared films exhibit layered structure through crosssection. Chemical composition analysis confirms that fluorine has been grafted onto grapheme scaffold through C—F covalent bond, and the doping level can be readily manipulated just by adjusting the reaction temperature. The structural changes of graphene induced by the controllable doping thus facilitate the tunable electrical property, which can be tuned over several orders of magnitude. These results indicate our method is not only potentially useful to tailor the chemical surface and electronic structure of graphene, but also can find applications in novel electronic devices based on graphene co-doped with different dopants.