Materials capable of dynamic persistent luminescence (PersL) within the visible spectrum are highly sought after for applications in display, biosensing, and information security. However, PersL materials with eye-detectable and excitation-wavelength-dependent characteristics are rarely achieved. Herein, a nonstoichiometric compound CaGaxO4:Bi (x < 2) is present, which demonstrates ultra-long, color-tunable PersL. The persistent emission wavelength can be tuned by varying the excitation wavelength, enabling dynamic color modulation from the green to the orange region within the visible spectrum. Theoretical calculations, in conjunction with experimental observations, are utilized to elucidate the thermodynamic charge transitions of various defect states, thereby providing insights into the relationship between Bi3+ emitters, traps, and multicolored PersL. Furthermore, the utility of color-tunable PersL materials and flexible devices is showcased for use in visual sensing of invisible ultraviolet light, multicolor display, information encryption, and anti-counterfeiting. These discoveries create new opportunities to develop smart photoelectric materials with dynamically controlled PersL for various applications.