Persistent luminescence (PersL) materials have attracted significant attention due to their unique ability to store photo-generated carriers and release them slowly, producing long-lasting emission after excitation ceases. However, the inherent limitation of single-color, single-mode emission in conventional systems severely restricts their information storage capacity and anti-counterfeiting security levels. To address this challenge, we developed a novel multicolor, multimode PersL material, BaGa₂Si₂O₈:Pr³⁺,Tb³⁺ (BGSO:Pr³⁺,Tb³⁺), through a rare-earth co-doping strategy, aiming to achieve effective separation of PersL and photoluminescence (PL) centers within a single host. A series of BGSO:Pr³⁺,Tb³⁺ phosphors were synthesized via a high-temperature solid-state reaction. Their crystal structure and morphology were characterized by XRD and SEM. The optical properties, including PL, PersL, thermoluminescence (TL), and photostimulated luminescence (PSL), were systematically investigated using spectral analysis, decay kinetics, and temperature-resolved measurements. Flexible PDMS films were also fabricated to evaluate potential information storage and encryption applications. The results confirm the successful incorporation of Pr³⁺ and Tb³⁺ into the BGSO lattice. Spectral analysis reveals distinct functional roles for the two dopants: Tb³⁺ acts as the dominant afterglow center, while Pr³⁺ serves almost exclusively as a PL center and lattice defect modulator rather than a trap center. This distinction enables effective separation of the afterglow and luminescence centers. TL measurements indicate a quasi-continuous deep-trap distribution (0.25&8211;0.63 eV) in the co-doped system. By mediating trap density and depth via doping, the material exhibits multimode fluorescence (PL, PersL, TL, and PSL) that can be dynamically controlled by temperature and near-infrared laser irradiation (808/980 nm). Notably, an abnormal thermal quenching phenomenon was observed, where the afterglow effect compensates for the high-temperature PL intensity. Leveraging these properties, we demonstrated high-throughput optical information storage with temperature-controlled readout, successfully encoding multi-level "plant growth" pa into traps of varying depths. In summary, this work presents a BGSO:Pr,Tb multimode fluorescent material with multicolor and multimode emission characteristics. It elucidates the intrinsic coupling mechanisms between rare-earth dopants and the host matrix, providing a theoretical foundation for designing advanced PersL, PSL, and TL materials. The findings offer a universal strategy for high-security optical encryption, complex information storage, and other emerging optoelectronic applications.