Long persistent luminescence materials developed to commercial standards are primarily concentrated in the blue and green regions, with only a few in the red region. Red, as one of the three basic colors, can be mixed in various proportions with blue and green to yield various colors. The development of red persistent phosphors has a broader application potential but remains a challenge. A solid-state reaction method was used to synthesize new red persistent luminescent materials of Ba 1- x Sr x Ga 2 O 4 :Sm 3+ ( x = 0–0.09). In BaGa 2 O 4 , both Sr 2+ and Sm 3+ preferentially occupy the Ba 2+ site rather than the Ga 3+ site. When exposed to UV light at 254 nm, the phosphors emit the characteristic red emission of Sm 3+ at wavelengths ranging from 500 nm to 750 nm. After removing the UV light source, an intense red afterglow that lasted more than 1400 s was observed. The red afterglow signal reappears after a heating process. Doping Sr 2+ reduces the trap depth and improves the red persistent luminescence significantly. Because the escaped electrons from traps compensate for the emission loss of Sm 3+ during the heating process, the red phosphors have unimaginably luminescent thermal stability. Thus, the emission intensity at 200 ° C is 1.6 times that at room temperature. The prepared red persistent phosphors show multimode luminescence, with the output signal being time and temperature sensitive, indicating that they are potential luminescent materials for anti-counterfeiting applications. Finally, a building-block strategy for advanced anti-counterfeiting applications of dynamic display information is proposed, with red persistent phosphors serving as an important component combined with upconversion phosphors of NaYF 4 :Yb 3+ , Tm 3+ , and green persistent phosphors of SrAl 2 O 4 :Eu 2+ , Dy 3+ .