Biomineralization‐Inspired Synthesis of Hybrid COF Nanosheets toward Efficient Desalination Membranes

Abstract Synthesis of covalent organic framework nanosheets (CONs) with high aspect ratio is crucial to their assembly into advanced membranes. Nonetheless, the π‐π stacking between covalent organic framework (COF) layers often leads to thick CONs. Herein, inspired by biomineralization process, a series of aspect ratio CONs >15 000 is synthesized by multifunctional polyelectrolytes which not only provide the nucleation sites for pre‐assembly with COF monomer, but also suppress π‐π interaction for anisotropic growth through protonation. The membrane assembled from CONs exhibited water permeance of 341 kg m −2 h −1 and salt rejection of 99.5% in desalination, outperforming ever‐reported membranes. This method establishes a platform for the synthesis of crystalline nanosheets.