There has been considerable interest in chemically functionalizing graphene films to control their electronic properties, to enhance their binding to other molecules for sensing, and to strengthen their interfaces with matrices in a composite material. Most reports to date have largely focused on noncovalent methods or the use of graphene oxide. Here, we present a method to activate CVD-grown graphene sheets using fluorination followed by reaction with ethylenediamine (EDA) to form covalent bonds. Reacted graphene was characterized via X-ray photoelectron spectroscopy (XPS), attenuated total reflectance Fourier transform infrared spectroscopy (ATR-FTIR), and Raman spectroscopy as well as measurements of electrical properties. The functionalization results in stable, densely packed layers, and the unbound amine of EDA was shown to be active toward subsequent chemical reactions.