A simple and efficient approach to endow the controllable multi-stimuli-responsive property for the supramolecular polymer was successfully developed by rationally introducing iodine into a novel naphthalimide-functionalized pillar[5]arene-based supramolecular polymer (PNA⊃GBP). Interestingly, by introducing iodine into the supramolecular polymer PNA⊃GBP, the iodine could not only control the optical properties and self-assembly states of PNA⊃GBP via electronic donor–acceptor effect but also control the molecular recognition properties by competitive redox reaction. Benefiting from these excellent iodine controlled multiresponse properties, the PNA⊃GBP showed selective fluorescent response for cyanide, cysteine, and mercury in supramolecular polymer gels, water solutions, and living cells with high sensitivities. The supramolecular polymer PNA⊃GBP could act as a novel smart material for selective detection CN–, Hg2+, and l-Cys.
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