The effective treatment of oily wastewater is of great significance for the protection of the ecological environment and human health. Aiming to prepare a membrane with excellent antifouling properties, a new active antifouling carbon cloth@Ni-Co LDH/Ag (CC@LDH/Ag) membrane was reported here via in situ hydrothermal growth and followed photo-deposition methods. The effects of Ag deposition on self-cleaning ability and surface wettability of CC@LDH/Ag membrane were studied. The experimental results showed CC@LDH/Ag membrane is superhydrophilic/underwater superoleophobic, and exhibited high separation efficiency (>98.6%) and high flux (6551–22,050 L m −2 h −1 ) for different kinds of oil/water mixtures. Moreover, CC@LDH/Ag membrane also displayed excellent environmental and mechanical durability. Good self-cleaning ability enabled CC@LDH/Ag membrane to be separated at least 30 times, and still maintained high separation performance. The self-cleaning CC@LDH/Ag membrane may hold great application prospects in oily wastewater remediation. A CC@LDH/Ag membrane with acicular hierarchal structure was constructed by in situ hydrothermal growth and followed photo-deposition methods. The CC@LDH/Ag membrane possessed outstanding separation efficiency with over 98.6% and high flux with range of 6551–22,050 L m −2 h −1 for multifarious oil/water mixtures. Moreover, CC@LDH/Ag membrane can be separated at least 30 times and still retained high separation performance, indicating a good self-cleaning performance. • A new active antifouling CC@LDH/Ag membrane via in situ hydrothermal growth and followed photo-deposition methods. • The CC@LDH/Ag membrane exhibited high separation efficiency and high flux for different kinds of oil/water mixtures. • Good self-cleaning ability enabled CC@LDH/Ag membrane to be separated at least 30 times. • The CC@LDH/Ag membrane displayed excellent environmental and mechanical durability.