In order to fabricate graphite nanosheets from graphite flakes, edge-functionalized graphite nanosheets were prepared by a functionalization method using phthalic acid as the molecule to be grafted. A polyphosphoric acid/P2O5 solution containing graphite and phthalic acid were heated at different temperatures for 72 h in a nitrogen atmosphere. It was confirmed by transmission electron microscopy and atomic force microscopy that the resultant phthalic acid-functionalized graphite nanosheets had a large surface area of 20.69 μm2 in average and an average thickness of 1.39 nm. It was also found by X-ray diffractometry and Fourier transform infrared spectroscopy (FT-IR) analysis that the functionalization caused the formation of C=O bonds at the edges of the graphite nanosheets. The yield from this functionalization method was found to be dependent on the reaction temperature, only when it is between 70 and 130°C, because of the dehydration of phthalic acid at higher temperatures. This was confirmed by FT-IR analysis and the observation of low thermal energies at low temperatures.