N-doped graphene aerogel with a three-dimensional interconnected network was fabricated by using graphene oxide and melamine via the hydrothermal self-assembly and thermal annealing process. The aerogels were characterized by means of scanning and transmission electron microscopy, Fourier transform infrared spectrum, X-ray photoelectron spectroscopy, elemental analyses, X-ray diffraction, Raman spectrum, and nitrogen adsorption/desorption measurement. The N-doped graphene aerogel showed high-specific surface area, superhydrophobic nature, excellent adsorption capacity for organic solvents, and adsorption recyclability. It would be a promising material for removal of organic contaminates from water.