Functionalized graphene aerogel with high porosity and hydrophobicity is prepared by surface modification of self-assembled graphene oxide aerogels. Fluorinated functional groups are introduced into the surface of three-dimensionally macroporous graphene aerogel through a one-step solution immersion method. Successful fabrication and surface modification of graphene aerogel are confirmed by various techniques. The functionalized graphene aerogel represents superior physical features, including low density (bulk density of 14.4 mg cm(-3)), high porosity (>87%), mechanical stability (supports at least 2600 times its own weight), and hydrophobicity (contact angle of 144 degrees. By combining the structural features and hydrophobic surface property, the functionalized graphene aerogel not only exhibits excellent absorption performance for various types of oils and organic solvents (capacity up to 11,200% of its weight), but also shows a remarkable regeneration capability (no obvious change in absorption capacity), making them an ideal candidate for eliminating spilled oils and other toxic organic pollutants. (C) 2015 Elsevier B.V. All rights reserved.