Although the fluorinated graphene (FG) possesses numerous excellent properties, it can not be really applied in aqueous environments due to its high hydrophobicity. Therefore, how to achieve hydrophilic FG is a challenge. Here, a method of solvent-free urea melt synthesis is developed to prepare the hydrophilic urea-modified FG (UFG). Some characterizations via transmission electron microscopy (TEM), atomic force microscopy (AFM), Fourier transfer infrared spectroscopy (FTIR), X-ray photoelectron spectroscopy (XPS), and thermo gravimetric analysis (TGA) demonstrate that the urea molecules can covalently functionalize the FG and the hydrophilic UFG can be prepared. According to the tribological tests run on an optimal-SRV-I reciprocation friction tester, it can be found that the antiwear ability of water can be largely improved by adding the appropriate UFG. When the concentration of UFG aqueous dispersion is 1 mg/mL, the sample of UFG-1 has the best antiwear ability with a 64.4% decrease of wear rate compared with that of the pure water (UFG-0), demonstrating the prepared UFG can be used as a novel and effective water-based lubricant additive.