Polymeric membranes have been widely studied and used in the field of water treatment because of their great chemical tolerance and ability to perform energetic separations. However, the inherent hydrophobicity of these materials has resulted in fouling issues that have hindered their development. It is critical to design hydrophilic antifouling membranes with micro/nano-structure through tailorable interface functionalization. Herein, a composite membrane with antifouling properties was prepared comprising of a hydrophilic tannic acid/polyvinylpyrrolidone (TA/PVP) composite layer and TiO minerals. The interfacial segregation process of TA was modulated to maximize exposed reaction sites for triggering subsequent interface mineralization. Density functional theory (DFT) calculations revealed that the molecular mechanism of TA/PVP inducing titanium dioxide nucleation. The optimal polyvinylidene fluoride (PVDF) membrane showed high pure water flux (587 L m h), superior bovine serum albumin (BSA) rejection (99.1 %) and a high flux recovery rate (91.9 %). The TA regulated interface mineralization strategy promises fabrication of multifunctional engineered materials towards water treatment, environmental remediation, and beyond.