Grafting fluorine onto graphene oxide (GO) by CF4 plasma treatment was investigated in this study. An easy, low-cost, and effective synthesis of the high-dispersive fluorinated GO (FGO) with tunable atomic ratio of F/O (R F/O) has been realized and the R F/O can be readily manipulated just by adjusting the reaction time. The influence of plasma treatment time on the microstructure, morphology, and dispersion of graphene nanosheets was systematically analyzed. X-ray photoelectron spectroscopy analysis confirmed that fluorine has been grafted onto graphene, and the R F/O was gradually increased to 3.54 for the FGO treated for 20 min. Morphology investigation indicated that etching on the edge of GO occurred during the fluorination. The dispersion performance of FGO in water reduced continuously, which in N,N-dimethylacetamide (DMAc) increased firstly and then decreased with the increase in plasma time. The zeta potentials of FGO in DMAc reached the lowest at −28.6 mV when GO was treated for 10 min. The dispersion of FGO in water should be attributed to the decrease of C–O group, while there was a same variation trend of FGO zeta potential in DMAc as the value of C–F content, regardless of R F/O, CF2 group content and CF3 group content. The GO film was super-hydrophilic and the film of FGO treated for 20 min was found to be neither hydrophilic nor hydrophobic.