In this study, ultralight and hydrophobic carbon aerogels were prepared from 2,2,6,6-tetramethyl-1-piperidinyloxy (TEMPO)-oxidized cellulose nanofibers (TOCN) for the removal of organic solvents. The morphology structure, density and chemical composition of TOCN aerogels freezed at -56°C and -196°C followed by pyrolysis were examined. The obtained carbon-based aerogels possessed ultralight density of 8.8 mg cm-3 and excellent fire-resistant property. The high porosity (up to 99.5%) and hydrophobic property (contact angle of 139.6°) of the obtained carbon aerogels allowed them to adsorb various organic solvents with high absorption capacity (up to 110-260 g/g). After five absorption-combustion and absorption-distillation cycles, the absorption capacity of TOCN carbon aerogels exhibited excellent recyclability with up to 64-99% of its initial absorption capability, demonstrating potential applications in oil-spill cleanup field.