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Naturally abundant vermiculite clay was expanded by using an aqueous solution of H2O2 and its surface was modified with ultra-thin polydimethylsiloxane (PDMS) using facile thermal vapor deposition to prepare an ecologically friendly, low-cost oil sorbent that plays an important role in oil spillage remediation. The resulting PDMS-coated expanded vermiculite (eVMT@PDMS) particles exhibited adequate hydrophobicity and oleophilicity for oil/water separation, with numerous conical slit pores (a size of 0.1–100 μm) providing a great sorption capacity and an efficient capillarity-driven flow pathway for oil collection. Simply with using a physically-packed eVMT@PDMS tube (or pouch), selective oil removals were demonstrated above and beneath the surface of the water. Furthermore, these sorbents were successfully integrated and then applied to the advanced oil-collecting devices such as a barrel-shaped oil skimmer and a self-primed oil pump.