To address oil spillage and chemical leakage accidents, the development of efficient sorbent materials is of global importance for environment and water source protection. Here we report on a new type of carbon nanofiber (CNF) aerogels as efficient sorbents for oil uptake with high sorption capacity and excellent recyclability. Importantly, the oil uptake ability of the CNF aerogels can be maintained over a wide temperaturerange,fromliquidnitrogentemperatureupto ca. 4006C,makingthemsuitableforoilcleanup under harsh conditions. The outstanding sorption performance of CNF aerogels is associated with their unique physical properties, such as low density, high porosity, excellent mechanical stability, high hydrophobicity and superoleophilicity.