The effective removal of oils and organic solvents from water is of great importance for environmental protection. Three‐dimensional nanofibrous aerogels (NFAs) with superabsorbent properties promise a huge potential applicability in oil spills and chemical leaks. However, the production of such NFAs through a facile and economical method is still a great challenge. Here, a very simple solution immersion process is presented to fabricate polydimethylsiloxane‐functionalized polyacrylonitrile NFAs. The obtained NFAs exhibit a superior chemical stability, a high hydrophobicity and an excellent absorption capacity for various oils and organic solvents. More importantly, these NFAs show an outstanding reversible elasticity and could potentially be employed for continuously collecting oils and organic pollutants from water with the assistance of a pump. It is believed that the obtained absorbents could be promising candidate materials for oil and organic solvent spill cleanups under harsh conditions.
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