The spillage of oil causes severe and long-lasting impacts on both the environment and human life. It is crucial to carefully reconsider the methods and techniques currently employed to recover spilled oil in order to prevent any possible secondary pollution and save time. Therefore, the techniques used to recover spilled oil should be readily available, highly responsive, cost-effective, environmentally safe, and, last but not least, they should have a high sorption capacity. The use of sorbents obtained from natural materials is considered a suitable approach for dealing with oil spills because of their exceptional physical characteristics that support sustainable environmental protection strategies. This article presents a novel sorbent material, which is a composite siloxane foam filled with bentonite clay, aimed at enhancing the hydrophobic and oleophilic behavior of the material. The thermal treatment of bentonite optimizes its sorption capacity by eliminating water, and increasing the surface area, and, consequently, its interaction with oils. In particular, the maximum sorption capacity is observed in kerosene and naphtha for the bentonite clay thermally treated at 600 °C, showing an uptake at saturation of 496.8% and 520.1%, respectively. Additionally, the reusability of the composite foam is evaluated by squeezing it after reaching its saturation point to determine its sorption capacity and reusability.