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Thin-film nanocomposites (TFN) nanomaterials have been employed to tailor permeability and selectivity in membranes, but achieving effective separation at large flux retains challenging. Here, the authors use calix[4]arene derivatives which are ionically bonded to a polyamide network to engineer the molecular-sieving properties of TFN membranes for organic solvent forward osmosis (OSFO).