Oil wastes pose an enormous threat to aquatic ecosystems, and environmental and economic demands emphasize the importance of affordable and sustainable oil absorbents. To tackle this issue, we propose the repurposing of abundant and low-cost cuttlebone from the ocean to address oil spills for the ocean. By the simple, successive deposition of polydopamine and a mixture of fluorinated silica nanoparticles and polydimethylsiloxane, the ultralight, porous, and mechanically stable cuttlebone is endowed with excellent superhydrophobicity and superoleophilicity. The as-obtained cuttlebone exhibits high absorption performance for various hydrocarbons and is successfully applied in a series of oil/water mixture separations. On this basis, an oil-collecting “cephalopod” electric device is designed by combining superhydrophobic/superoleophilic cuttlebone with a pumping system, and demonstrates excellent collection efficiency and recyclability for oil spill cleanup. This work provides a valuable perspective on the development of high-performance oil absorbents derived from sustainable natural marine products.