PersL is a unique phenomenon that a material emits for an appreciable time (seconds, minutes, hours, or days) after switching off an optical excitation. Without the requirement of a continuous optical excitation, persistent phosphors in the visible and infrared ranges have been extensively studied during past decades and have shown a vast range of promising applications underlying the "persistence" feature, including night-vision displays, [22] bio-imaging, [23,24] and optical information storage. [25] Not until recently have UVC persistent phosphors been found with promising applications in optical communication for all lighting conditions for the first time, with Pr 3+ as the UVC PersL ion. [26] Due to the complete absence of UVC solar radiation in the lower atmosphere, UVC PersL can be visualized free of any disturbance from outdoor lighting or artificial lights. Thus, UVC PersL from phosphors can satisfy a pointing and tracking function independent of ambient lighting conditions. Additionally, persistent photocatalysis, [27] persistent sterilization, [28] self-sustained imaging technique, [26] and other UV-sensitive or UV-stimulated applications [29,30] will be possibly achieved. These promising applications are beyond the expectations from phosphors with visible or infrared PersL.However, the development of UVC and UVB persistent phosphors is encumbered by the foreseeable difficulties. First, selecting an appropriate luminescence ion emitting at UVC and UVB spectral range is required. Pr 3+ is a well-suited luminescence ion with a UV-emissive 4f5d energy level for this purpose. [26] Based on that, UVC and UVB PersL can be achieved within a crystal host only with effective trapping centers to form UV-trapping energy levels. Unfortunately, the exact characteristics of trapping centers remains unclear even for many visible and infrared persistent phosphors using popular host materials such as aluminates, [31,32] gallates, [22][23][24] garnets, [33] and others. [25,34,35] The creation of traps in these phosphors may be varied from lanthanide codoping, [31] Li + doping, [36] and cationic substitution. [22,33] Garnet is a crystal structure in a generic chemical formula {A} 3 [B] 2 (C) 3 O 12 , consisting of linked [AO 8 ], [BO 6 ], and [CO 4 ] polyhedra. It is one of the most studied host matrixes accommodating lanthanide ions or transition metal ions due to its chemical and physical stability and tolerant nature for cationic substitution. [37][38][39][40] Cationic substitution or heterovalent cosubstitution at its A, B, and/or C Persistent luminescence (PersL) at the high-energy spectral end (ultraviolet, UV) is generally hard to achieve, although a long-lasting UV PersL can play an irreplaceable role in outdoor imaging and other UV-triggered applications. No PersL with dual ultraviolet C (UVC) and ultraviolet B (UVB) bands from a single material has previously been attained until the authors have designed Pr 3+ -doped (Ca 1.5 Y 1.5 )(Al 3.5 Si 1.5 )O 12 (CYAS-Pr) through cosubstituting Ca 2+ -Si 4+ into Y 3 Al 5...