AbstractHydrophobic membranes have been considered as one of the most effective candidates in oil/water separation for their easy operation and high efficiency. Here, we prepared a hydrophobic carbon nanotube (CNT)/carbon nanofiber (CNF) hybrid membrane by in situ grafting CNTs on a CNF membrane. The CNT grafting significantly increased the porosity and hydrophobicity of the CNF membrane. As a result, the CNT/CNF hybrid membrane showed a high efficiency (80%–98%) in the separation of a range of oil/water mixtures. Moreover, the CNT/CNF hybrid membrane is recyclable, and the separation efficiency maintained after 10 cycles. This high separation efficiency and good recyclability provide feasibilities for practical applications of the CNT/CNF hybrid membrane in the purification of oil contaminated water.