Polyurethane (PU) sponge has become a preferred oil adsorbent in recent oil-spill accidents. To make the sponge superhydrophobic and superoleophilic, this study used graphene (GN), which was modified with c-methacryloxypropyl trimethoxy silane (KH-570), to coat the PU sponge (called the KH-GN sponge). This study showed the best loading capacity (11.96%) of the KH-570modified GN on the sponge. The contact angles of the KH-GN PU sponge were 161 for water and 0 for soybean, diesel, and pumping oil. It had good selectivity for oil over water, and the KH-GN sponge achieved adsorption equilibrium within a few seconds. The absorption capability of the KH-GN sponge was up to 39 times greater. Additionally, the KH-GN PU sponge could be reused for oil-water separation for more than 120 cycles without losing its superhydrophobic and superoleophilic properties. Therefore, the sponge prepared in this study could be a desirable material for the cleanup of oil spills. V C 2015 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2015, 132, 41821.