Membrane filtration technology has been considered as a promising alternative for produced water treatment. However, membrane fouling is a critical problem that affects wastewater treatment efficiency. Membrane surface modification has been regarded as an effective method to improve membrane antifouling ability. In this study, a novel membrane surface modification method was proposed to obtain a super-hydrophilic membrane with high water permeability and great oil rejection through cold plasma-induced PAA graft-polymerization followed by nano-ZnO self-assembly. The results indicated that a PAA layer was uniformly formed on the membrane surface, and ZnO nanoparticles (NPs) were strongly immobilized by the PAA layer. The firm PAA-ZnO coating on membrane surface brought about dramatically improvements of membrane performances both in permeation flux and pollutant rejection rate.