Solvent‐Controlled Construction of Charge‐Transfer Solid‐State Supramolecular Polymers and Their Application in Selective Pyridine Vapor Detection

ABSTRACT This study employs a solvent‐directed strategy to construct organic charge‐transfer (CT) supramolecular polymers in the solid states. By utilizing clamparene ( CLP ) and 4‐nitrobenzonitrile ( NBN ) as building blocks, we achieved topologically controlled self‐assembly in different solvents. Specifically, in acetonitrile (CH 3 CN), strong π–π stacking mediated CT interactions facilitated the formation of a supramolecular polymer in the solid state, which exhibits a selective chromogenic response to pyridine (Py) vapor. This solvent‐modulated assembly approach not only enables the construction of functional CT supramolecular polymers with controllable topology but also provides a new pathway for designing vapor‐responsive materials.