A robust and simple method is provided to fabricate Janus polymer/carbon nanotube (CNT) hybrid membranes for oil/water separation. Starting from CNT membranes formed by dispensing, hydrophobic poly(styrene) (PS) and hydrophilic poly(N,N-dimethylaminoethyl methacrylate) (PDMAEMA) were grated from different sides of the photoactive CNT membranes via self-initiated photografting and photopolymerization (SIPGP) to achieve Janus polymer/CNTs hybrid membranes. The obtained membranes have excellent oil/water selectivity in the removal of oil from water. Moreover, they can effectively separate both surfactant-stabilized oil-in-water and water-in-oil emulsions because of the anisotropic wettability of the membranes.