A new unsymmetric diarylethene derivative 1-{4-(5-methoxy-2-(2-pyridyl)thiazolyl)}-2-{3-(2-methylbenzo-[b]thiophenyl)}hexafluorocyclopentene (1) was designed and synthesized. Fluorescence behaviors of 1 are multiswitched through protonation, coordination, and photochemical reactions due to the existence of multiple binding sites. Thus, the cooperation of chemical and optical input signals cascades several fundamental logic gates within the open form (1O) or closed form (1C) of 1, and the logic functions in 1O and 1C are reversible with photo-switch. Furthermore, photo-switch reversibly reconfigures logic functions from an INHIBIT logic gate (1C) to a half-subtractor (1O).

Inorganic–organic composite films for rewritable optical storage are fabricated base on the reversible luminescence modulation of ordered upconversion nanopatterns via a photochromic diarylethene. The near‐IR excitation for reading the upconversion emission does not affect the recorded data bits. Moreover, the spatially well‐defined 2D nanopatterns promise future applications in ultrahigh‐density storage.