Three-dimensional, cost-effective, and renewable/recyclable absorbent materials with high capacities on absorption of organic compounds are urgently in demand. Herein, a facile while innovative approach is reported to develop ultralight electrospun cellulose sponge (UECS). The prepared UECS exhibits super-high absorption capacity (up to 232 times of its own weight) towards absorption of organic compounds due to high porosity (99.57%), low density (6.45 mg/cm(3)), and hydrophobic surface feature (with water contact angle of 141.2 degrees). Furthermore, the UECS is mechanically robust thus can be readily cut into different shapes; and it also possesses excellent stability against various organic compounds. Intriguingly, upon absorption of an organic compound, the shape-stable UECS organic gel can be formed. Hence, the developed UECS would be promising as environmental friendly absorbent on high-performance separation of organic compounds from aqueous systems; while the UECS organic gel could be utilized for the applications such as drug delivery and sensor.