Surface modification of membranes using hydrophilic nanoparticles has proved promising to improve the surface wettability and antifouling properties of the membranes that are otherwise prone to the attachment of oil droplets. Nonetheless, the strong adhesion of nanoparticles onto the membrane surface and their long-term performance pose problems for their widespread application. To address these issues, a novel organic-inorganic hybrid coating was constructed onto surfaces of polyphenylsulfone (PPSU) ultrafiltration membrane via simultaneous deposition of mussel-inspired polydopamine (PDA) followed by immobilization of tannic-acid functionalized cerium oxide (CeO2) nanoparticles. These prepared membranes were characterized by FTIR, XPS, FESEM, EDX, pore size, water contact angle (WCA), underwater oil contact angle (UOCA), and separation performance. The effects of functionalization and nanoparticle concentration on membrane properties were investigated. SEM and EDX results showed that functionalized nanoparticles (up to optimum concentration: 0.05 wt%) were uniformly distributed onto the membrane surface, which exhibited increase in permeate flux (∼375 %), UOCA (∼36 %), Fouling resistance ratio (FRR ∼ 300 %) with a decrease in irreversible fouling (∼94 %) and WCA (∼80 %) and high oil rejection of > 99 % compared to pristine PPSU membrane. Long-term operation (for six cycles) indicates that the optimum membrane possessed high efficiency and durability for oil-in-water emulsion separation due to superb antifouling properties and strong binding of the functionalized nanoparticles onto the membrane surface.