Two-dimensional (2D) inorganic nanomaterials have garnered extensive attention in the fabrication of inorganic nanofiltration membranes due to their unique structures and properties. In this study, we developed a facile process for fabricating large-scale ultrahydrophilic nanofiltration membranes using layered titanate H1.07Ti1.73O4·nH2O nanosheets (HT-ns). A drying deposition process was used to fabricate HT-ns membranes on a poly(tetrafluoroethylene) (TF) substrate. To enhance the bonding strength between the substrate and the deposited HT-ns membrane, the substrate surface was modified with a Cu2+-adsorbed silane monomolecular layer, connecting a negatively charged HT-ns membrane and a positively charged substrate surface. The fabricated HT-ns membrane exhibited an excellent rejection performance for inorganic salts and dye molecules. The ultrahydrophilicity of HT-ns membrane with a low water contact angle of 31° results in an ultrafast water permeance, which is approximately 6 times higher than that of a simple graphene-based nanofiltration membrane. The results open a new avenue to a new category of ultrahydrophilic nanofiltration membranes.