In order to effectively clean oily seawater with anionic polyacrylamide (APAM), UiO-66 coated γ-Al₂O₃ (UA) composites were firstly synthesized using γ-Al₂O₃ as a template to induce the growth of high hydrophilic UiO-66 on its surface to form a uniform UA self-assembled membrane. The UA composites and self-assembled membrane were characterized and analyzed. Also, the membrane performance was investigated. The results show that the hydrophilicity of particles is enhanced with the water contact angle decreasing from 39.8° (γ-Al₂O₃ particles) to 26.2° (UA composites) by introducing the UiO-66 coating. Moreover, the UA self-assembled membrane performs attractive water yield and separation performance. The oil concentration in the permeate treated by the first class of UA self-assembled membrane declines apparently from 91.22 to 18.90 mg L⁻¹, while the water yield is as high as 657.89 L m⁻² h⁻¹. The reclaimed separation experiments show that the membrane materials could be recycled by calcination at 200 °C and hydraulic cleaning, which gives the material potential application in cleaning oily seawater.