AbstractThe increasing water pollution problem poses a demand for oil–water separation materials, but preparing separation materials with high efficiency and excellent durability remains a great challenge. In this work, we use a diblock polymer brush of polydimethylsiloxane (PDMS) and poly(N,N‐dimethylaminoethyl methacrylate) (PDMAEMA) based on cotton fabric to prepare oil–water separation membranes with high efficiency, good durability, and intelligent self‐repairing properties. Lubricating PDMS brushes reduces the fouling adhesion due to its low surface energy and high flexibility. pH‐responsive PDMAEMA brushes provide good hydrophobicity and an intelligent self‐repairing effect. The prepared Co‐PDMS‐PDMAEMA has high oil flux (>30,000 L m−2 h−1) and high separation efficiency (>99%) even after 10 cycles and its surface character can be recovered under acidic conditions. Overall, the modified cotton fabric made by such a versatile technique is promising in oil–water separation.