Separation and purification on molecular level from organic solvent mixtures are of paramount importance in industries. Organic solvent nanofiltration (OSN) is a pressure‐driven membrane separation process providing an attractive alternative to conventional energy‐intensive technologies. However, devising a solvent stable, scalable membrane with high permeability and excellent selectivity is still a challenge. Interfacially polymerized thin‐film composite (TFC) OSN membranes integrating an ultrathin selective layer and a porous substrate layer are expected to revolutionize advanced membrane separations. New materials and new strategies to achieve a solvent resistant, highly permeable, and highly selective membrane have been developed in recent years. This review analyses the development of the state‐of‐the‐art interfacially polymerized TFC OSN membranes from the view of structures, materials, and methodologies. First, the emerging structures of current TFC OSN membranes are discussed. The exploitation of new materials (polymers, (nano)fibers, inorganic materials) for the preparation of substrate layer is updated. The advances of new aqueous/organic monomers for synthesis of the selective layer are summarized. Furthermore, the proposed strategies for designing permselective TFC membranes are highlighted. Finally, the challenges together with the future prospects of interfacially polymerized TFC membranes for OSN are proposed.