Oil spill accidents contaminate the oceanic environment and cause economic distress, and they continue to occur. Many methods have been developed to restore waters contaminated with spilled oil. However, still most commercially available methods are not environmentally or economically sustainable solutions. Therefore, there is a need for the development of sustainable materials with running water treatment capabilities. In recent years, a polyurethane (PU) sponge-based adsorbent has been reported as an oil–water separation and reusable adsorbent. This is because the porous 3D structure of the PU sponge provides a large surface area. However, as the PU sponge has a carboxyl group and an amino group, it exhibits hydrophilicity, so surface modification is essential for oil–water separation. Therefore, to modify the surface of PU to have hydrophobic/oleophilic properties, a hydrophobic/oleophilic adsorbent (HOA) was prepared using graphite and polydimethylsiloxane. On the basis of this, a PU sponge, a porous material, was used to manufacture an adsorbent that can be used in a sustainable and environmentally friendly way. The prepared HOA can selectively adsorb water or oil and can be reused. Furthermore, continuous oil–water separation is possible through a simple flow of fluid. Therefore, it is confirmed that the studied HOA can have great potential for ocean restoration in the future as an adsorbent that mitigates the disadvantages of the currently commercialized method.