Aerogel has excellent application potential in adsorption, heat preservation, and other areas due to its typical advantages of low density and high porosity. However, there are several issues with the use of aerogel in oil/water separation, including weak mechanical qualities and challenges in eliminating organic contaminants at low temperature. Inspired by cellulose Iα, which has excellent performance at low temperature, this study used cellulose Iα nanofibers extracted from seaweed solid waste as the skeleton, through covalent cross-linked with ethylene imine polymer (PEI) and hydrophobic modification of 1, 4-phenyl diisocyanate (MDI), supplemented by freeze-drying technology to form three-dimensional sheet, and successfully obtained cellulose aerogels derived from seaweed solid waste (SWCA). The compression test shows that the maximum compressive stress of SWCA is 61 kPa, and the initial performance still maintains 82% after 40 cryogenic compression cycles. In addition, the contact angles of water and oil on the surface of the SWCA were 153° and 0°, respectively, and the stable hydrophobic time in simulated seawater is more than 3 h. By combining the elasticity and superhydrophobicity/superoleophilicity, the SWCA with an oil absorption capacity of up to 11–30 times its mass, might be utilized repeatedly for the separation of an oil/water mixture.