Highly porous nanocellulose aerogels can be prepared by vacuum freeze-drying from microfibrillated cellulose hydrogels. Here we show that by functionalizing the native cellulose nanofibrils of the aerogel with a hydrophobic but oleophilic coating, such as titanium dioxide, a selectively oil-absorbing material capable of floating on water is achieved. Because of the low density and the ability to absorb nonpolar liquids and oils up to nearly all of its initial volume, the surface modified aerogels allow to collect organic contaminants from the water surface. The materials can be reused after washing, recycled, or incinerated with the absorbed oil. The cellulose is renewable and titanium dioxide is not environmentally hazardous, thus promoting potential in environmental applications. © 2011 American Chemical Society