Thin-film composite (TFC) membranes are commendable semipermeable barriers for water treatment. Although conventionally immiscible interfaces between aqueous and organic solutions are widely utilized for obtaining TFC membranes, interfacial polymerization still suffers from the issues of harmful solvents, complex diffusion/ reaction of the reactants, and thermodynamic and kinetic instability of interfaces. In this study, vapor-phase polymerization with no requirements for organic solvent and immiscible interface is utilized for processing TFC nanofiltration membranes. Through cross-linking of β-cyclodextrin and piperazine layers by trimesoyl chloride vapor, polyester and polyamide TFC membranes with high cross-linking degree are simply prepared in a scalable and reproducible manner. The prepared TFC membranes exhibit stable nanofiltration and desalination performance for all water, organic solvent, and water-organic mixture systems, with permeance up to an order of magnitude higher than that of commercial membranes.