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Two complexes based on phosphorescent viologen ligands have been synthesized. Complexes 1 and 2 not only possess reversible photochromic and electrochromic properties, but also exhibit fluorescence and persistent luminescence. They have potential applications in inkless print, color-changing films, data encryption, and anti-counterfeiting. [Display omitted] • Complexes 1 and 2 exhibit reversible photochromic and electrochromic behaviors. • Complexes 1 and 2 exhibit long-lived persistent phosphorescence. • Complexes show great potential in data encryption and anticounterfeiting. • Complexes have potential applications in inkless printing, color-changing films. Viologen-based complexes have garnered significant attention due to their multifunctional stimuli-responsive properties and tunable persistent luminescence. However, achieving ultralong afterglow emission and color change in these complexes remains a challenge, limiting their application in the field of persistent luminescence. Herein, two novel viologen-based complexes were successfully designed and synthesized using N,N′-bis(2-carboxyethyl)-4,4′-bipyridinium dichloride (H 2 bybpy) ligands and trimesic acid (H 3 BTC) with the transition metals Zn(II)/Cd(II). Complexes 1 and 2 display reversible photochromic and electrochromic properties. Interestingly, complexes 1 and 2 in their crystal state exhibit dual fluorescence and persistent luminescence, emitting a green and cyan afterglow when the UV lamp is turned off at 77 K. Incorporating phosphorescent molecules and changing the metal significantly extended the duration of persistent luminescence and altered the hue. The complexes were also demonstrated to have potential applications in inkless printing, color-changing films, data encryption, and anti-counterfeiting. This work enhances the application of viologen-based complexes in light-controlled persistent fluorescence and provides ideas for achieving ultra-long afterglow emission. [ABSTRACT FROM AUTHOR]