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The development of new sensors for the accurate detection of cyanide anion has attracted more and more attention due to their potential applications in environmental and biological systems. Here, two novel near‐infrared (NIR) photochromic compounds 1a and 1b, which were modified by the dicyanovinyl fragment with cyanide recognition function, have been developed. Surprisingly, 1a presented an unprecedented triple sensing performance for cyanide anion (colorimetric‐fluorescent‐colorimetric), which can be utilized as a potential precision sensor for CN– in environmental and biological systems. Although 1b did not show triple detection behavior for CN–, it could recognize CN– and F– synchronously and selectively by naked eyes. Moreover, their NIR photochromic behaviors could be modulated by the cyanide anion. Their sensing mechanism for CN– or F– was confirmed by absorption spectral studies, NMR titration, and DFT calculations. [ABSTRACT FROM AUTHOR]

A series of novel dithienylethene-based colorimetric sensors 1a-1d with a typical donor-acceptor structure have been successfully developed, which exhibited solvent-dependent photochromic properties in solution, as well as high selectivity and sensitivity for the naked-eye detection of cyanide anion in 95% aqueous CH 3 CN media. Moreover, it was found that different structures had a noteworthy effect on both their photochromic properties and colorimetric sensing for CN−. The sensing mechanism based on the nucleophilic addition reaction with CN− was confirmed by absorption spectral studies, 1H NMR titration and DFT calculations. Among them, the sensor 1b displayed highly sensitive to CN− (35 s) and lower detection limit (0.25 μM), which can be utilized as a potential colorimetric sensor for CN− in our daily life and environment. Image 1 • A series of novel dithienylethene-based colorimetric sensors were developed. • They exhibited solvent-dependent photochromic properties in solution. • They displayed the naked-eye detection of CN− with high selectivity and sensitivity. • Different structures had a noteworthy effect on both their photochromic properties and colorimetric sensing for CN−. • 1b displayed highly sensitive to CN− and lower detection limit. [ABSTRACT FROM AUTHOR]