This paper reports the optimization of a two-step atmospheric pressure plasma process to modify the surface properties of a polyurethane (PU) foam and, specifically, to prepare a superhydrophobic/superoleophilic absorbent for the removal of oils and nonpolar organic solvents from water. In particular, in the first step, an oxygen-containing dielectric barrier discharge (DBD) is used to induce the etching/nanotexturing of the foam surfaces; in the second step, an ethylene-containing DBD enables uniform overcoating with a low-surface-energy hydrocarbon polymer film. The combination of surface nanostructuring and low surface energy ultimately leads to simultaneous superhydrophobic and superoleophilic wetting properties. X-ray photoelectron spectroscopy, scanning electron microscopy and water contact angle measurements are used for the characterization of the samples. The plasma-treated PU foam selectively absorbs various kinds of hydrocarbon-based liquids (i.e., hydrocarbon solvents, mineral oils, motor oil, diesel and gasoline) up to 23 times its own weight, while it completely repels water. These absorption performances are maintained even after 50 absorption/desorption cycles and after immersion in hot water as well as acidic, basic and salt aqueous solutions. The plasma-treated foam can remove mineral oil while floating on the surface of mineral oil/water mixtures with a separation efficiency greater than 99%, which remains unaltered after 20 separation cycles.