Organic solvent nanofiltration (OSN) is an effective technology for separating solute with molecular weight of 200–1000 Da (Da) from organic solvents. However, as the core of this technology, most of OSN membranes exhibit a low solvent permeance. Herein, a highly permeable OSN membrane was prepared via a poly (sodium 4-styrenesulfonate) (PSSNa)-assisted interfacial polymerization reaction using ultra-low content of aqueous monomer solution, followed by a protective modification using tannic acid (TA) grafting onto the nascent polyamide surface, and a post chemical crosslinking treatment as well as an activation treatment. PSSNa manipulates the diffusion and distribution of the m-Phenylenediamine monomers, leading to a looser and thinner polyamide layer. TA molecules successfully reacted with the remaining acyl chloride groups on the nascent polyamide layer surface and formed ester, thus preventing the surface from subsequent crosslinking reaction and also making the selective layer looser, which is beneficial for solvent permeation. Moreover, the TA modification makes the surface more hydrophilic, thus further helps to improve the solvent permeance of OSN membrane. The optimal membrane possesses an excellent ethanol permeance of 71.5 L m−2 h−1 MPa−1, an increment of 41.6 % as compared with the baseline OSN membrane, while keeping a rejection of 98.2 % for rhodamine B (RDB). Meanwhile, the surface of optimal membrane is ultra-smooth, with an average roughness of 4.4 nm, which is much beneficial for antifouling. Moreover, the OSN membrane possesses a brilliant durability performance, with only a 1.5 % decrease of the RDB rejection after being immersed in N, N-Dimethylformamide (DMF) at room temperature for 115 d, and only a further 0.3 % decrease of the RDB rejection after being further immersed in DMF at 80 °C for another 11 d, indicating its superior solvent resistance, which makes it a promising candidate for treating organic solutions from pharmaceutical and textile industries.

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