The facile method to functionalize graphene oxide through surface modification with acetone was studied and improved. The resulting nanomaterials showed variable characteristics as the surface energy could be tailored according to the combination (proportion of H2O to acetone) of mixed solvent under sonication. Stability test and contact angle measurement showed that the treated graphene oxide exhibited different dispersibility and wettability. SEM images of graphene oxide films corroborated the changes in chemical composition of the sheets. FT-IR, XPS, and TGA observation provided direct evidence for chemical composition changes occurred on the surface. The presence of alkyl chain could decrease the surface energy and obviously control the hydrophilicity of the graphene oxide sheets. These results will provide significant guidance for the study of graphene-based bio-materials and nano-composites.