Reduced graphene oxide (rGO) was covalently bound onto the surface of polyurethane (PU) sponge using two different coupling agents: (3-aminopropyl)triethoxysilane and titanium(IV)(triethanolaminato)isopropoxide. The coupling agents were introduced before and after reduction of graphene oxide to compare the impact of the sequence on the absorbance capacities. The sponges were evaluated based on hydrophobicity and pump oil absorbance capacities. The structure and properties of the sponges were evaluated using scanning electron microscopy and Fourier transform infrared spectroscopy. Results revealed that reacting the graphene oxide PU sponge with the coupling agent titanium(IV)(triethanolaminato)isopropoxide prior to reduction significantly improved oil absorbance. This was due to the improved binding of reduced graphene oxide to the polyurethane framework. The resulting improved rGO-coated PU sponge is a highly efficient and reusable sorbent material and is a promising alternative for oilwater separation applications.