Graphene aerogels (GAs) are increasingly being recognized as high performance multifunctional materials to tackle our current and emerging environmental concerns. In order to extend the application potential of GAs, herein we have successfully synthesized nitrogen (N) and sulfur (S) codoped GAs (NSGAs) via a simple, scalable, and inexpensive approach. Owing to their large specific surface area (up to 132 m2 g-1), profound porosity, superior mechanical properties, and coexistence of N and S atoms with tunable atomic content and bonding configurations, the as-prepared NSGAs demonstrated exceptional absorption capacity toward a broad spectrum of oils and organic solvents, with an average absorption rate many folds higher than conventional absorbents. Further, the NSGAs exhibited excellent photocatalytic activity for the decomposition of recalcitrant organic compounds under visible light illumination due to pronounced synergistic coupling effect between the heteroatoms. Specifically, after 5 h of exposure to visible light, a degradation efficiency of over 99% was observed and more than 84% of the total organic carbon was eliminated. Radical trapping experiments revealed that superoxide anion radicals are the predominant oxygen reactive species driving the photocatalytic reactions. More importantly, the mineralization byproducts did not pose any significant antibacterial activity, illustrating the environmentally benign nature of these macroscale photocatalysts.