LAUSR

Supramolecular metal‐organic materials are considered as the ideal candidates for membrane fabrication due to their excellent film forming characteristics, diverse metal centers and ligand sources, and designable structure and function. However, it remains challenging to rapidly construct highly permeable supramolecular metal‐organic membranes with high salt rejection. Herein, a novel ultrafast interfacial self‐assembly strategy to prepare supramolecular metal‐organic films through the strong coordination interaction between highly active 1,3,5‐triformylphloroglucinol (TFP) ligands and Fe3+, Sc3+, or Cu2+ at the organic–aqueous interface is reported. Benefiting from the self‐completing and self‐limiting characteristics of this interfacial self‐assembly, the new kind of supramolecular membrane with optimized composition can be assembled within 3.5 min and exhibits ultrathin, dense, defect‐free features, and thus shows an excellent water permeance (21.5 L m–2 h–1 bar–1) with a high Na2SO4 rejection above 95%, which outperforms almost all of the non‐polyamide membranes and commercially available nanofiltration membranes. This strong‐coordination interfacial self‐assembly method will open up a new way for the development of functional metal‐organic supramolecular films for high‐performance membrane separation and beyond.