Dopamine chemistry arising from marine mussel bioadhesion principles has attracted growing interest in designing and fabricating robust thin films/membranes for various chemical separation processes.

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Thin-film nanocomposite membranes have shown great promise in organic solvent nanofiltration. However, it is challenging to acquire high permeation flux without severe swelling, which might do harm to rejection and long-term stability. In this study, we introduced dopamine-modified mesoporous silica nanoparticles into the polyamide (PA) matrix via interfacial polymerization to fabricate a series of thin-film nanocomposite membranes. By using polyethyleneimine (PEI) as the aqueous monomer, the modified nanoparticles are designed to be cross-linked within the PA network, which allows the penetration of PEI into the mesopores, and therefore, the membranes show better resistance to solvent-induced swelling and pressure-induced densification. More importantly, the mesopores of nanoparticles provide additional fast channels for solvents, resulting in an unusual enhancement of solvent flux under reduced membrane swelling. Along with the permeation flux, the rejection performance of the nanocomposite membranes is simultaneously improved, thanks to the controlled swelling arising from the strong interfacial adhesion. Thin-film nanocomposite membranes with optimal filler concentration exhibit a high isopropanol permeance of 8.47 L m −2 h −1 bar −1 as well as a quite low-molecular-weight cutoff of 281 Da.