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Fluorescent photochromic molecules that exhibit distinct light‐triggered changes in their emission colors are highly desirable for the fabrication of smart soft materials and advanced photonic devices. α‐Cyanodiarylethenes, that is, α‐cyano‐functionalized diarylethenes, as alternative “non‐azo” Z/E photochromic molecular switches, are popular choices due to their unique characteristics such as their aggregation‐induced emission or aggregation‐induced‐enhanced emission behavior in their self‐assembled states, and visible changes in fluorescence colors during Z/E photoisomerization. In recent years, the development of fluorescent photochromic α‐cyanodiarylethene‐based compounds including α‐cyanostilbenes, dicyanodistyrylbenzenes, and diaryldicyanoethenes, has mainly focused on molecular design, photochemical and photophysical behavior in solution, and smart soft matter technologies. In this review, recent significant achievements in light‐responsive systems based on the Z/E photoisomerization of fluorescent photochromic α‐cyanodiarylethene switches that span the range from liquid crystals to gels and finally to self‐assembled nanostructures, are highlighted. The smart soft materials constructed from α‐cyanodiarylethene molecular switches find use in a plethora of areas, including display, sensing, encrypting, actuating, and biomedical imaging applications, among others. The review concludes with a brief perspective on some major challenges and opportunities for the future development of light‐responsive smart soft photonic materials.

Optically reconfigurable monodisperse chiral microspheres of self-organized helical superstructures with dynamic chirality were fabricated via a capillary-based microfluidic technique. Light-driven handedness-invertible transformations between different configurations of microspheres were vividly observed and optically tunable RGB photonic cross-communications among the microspheres were demonstrated.