phototoxicity and drawbacks of traditional UV light excitation due to low-penetration. [6] Recently, breakthroughs have been made in azobenzene-based photochromic materials, as high thermostability and all-visible light-controlled azobenzenes have been successively developed via ortho-/para-substitution, [7] multiphoton sensitization [8] as well as introducing new aryl groups. [3b,9] Various applications based on these newly designed azobenzenes have also been reported. [10] Correspondingly, as a promising P-type photochromic material, [11] diarylethene (DAE) derivatives have encountered an obstacle in extending their excitation range from ultraviolet to all visible area with high efficiency and good photorobustness. Though the association of DAEs with multiphoton excitation, [12] upconversion nanoparticles, [13] and metal-to-ligand charge transfer (MLCT) [14] has been applied to induce photochromism with visible light, strategy for all-organic (or metal-free), visiblelight photochromism of DAEs is rather limited. The strategy reported till now is mainly focused on the elongation of the aryl moiety conjugation to red-shift the absorption of the open isomer. [15] Irie and co-workers successfully synthesized a visible photochromic DAE derivative by introducing perylene monoimide into the reaction carbon site of the thiophene moiety. [15a] Hecht and co-workers extended the conjugation of DAE with triplet sensitizer biacetyl, which achieved both visible-light photochromism and high fatigue resistance via triplet-triplet energy transfer (TTET) manifold. [15b] Nonetheless, conjugation extension would decrease the contribution of the excited singlet state of the central hexatriene moiety, which in some cases indeed suppresses the photochromism. [15,16] As a result, elaborate structural design is essential for DAEs with both visible-light photochromism and good performances, which might lead to tedious synthesis and unpredictable performances. To overcome these ever-emerging obstacles, developing new design strategies for photochromic DAEs becomes more and more imperative.Photocyclization of DAEs via triplet excited state (T 1 ) energy transfer from a triplet sensitizer has been proved to be available for ring closure and high fatigue resistance. [1a] Besides, the relatively low-lying T 1 of DAE open isomer offers a possibility for photochromism with longer excitation wavelength. Unlike the favorable MLCT effect which is based on diverse transition metal complexes (e.g., Ru, Os, Re, and Ir), [14] metal-free triplet sensitizers do not reach their potential in visible-light All-organic visible-light photochromism is reported here via a novel strategy with narrow singlet-triplet energy gap (ΔE ST ) materials as a sensitizer. Taking advantage of the narrow ΔE ST feature and the triplet-triplet energy transfer process, highly efficient photochromism of diarylethenes (DAEs) with both ring-open and ring-closure excitations shifted to visible light region is successfully achieved. Moreover, the wavelength of the visi...