Developing X-ray or UV-light charged storage and mechanoluminescence (ML) materials with high charge carrier storage capacity is challenging. Such materials have promising utilization in developing new applications, for example, in flexible X-ray imaging, stress sensing, or non-real-time recording. Herein, the study reports on such materials; Bi 3+ , Tb 3+ , Ga 3+ , or Ge 4+ doped LiTaO 3 perovskite storage and ML phosphors. Their photoluminescence, thermoluminescence (TL), and ML properties are studied. The charge carrier trapping and release processes in the Bi 3+ , Tb 3+ , Ga 3+ , or Ge 4+ doped LiTaO 3 are explained by using the constructed vacuum referred binding energy diagram of LiTaO 3 including the energy level locations of unintended defects, Tb 3+ , Bi 3+ , and Bi 2+ . The ratio of the TL intensity after X-ray charging of the optimized LiTaO 3 :0.005Bi 3+ ,0.006Tb 3+ ,0.05Ga 3+ , or LiTaO 3 :0.005Bi 3+ ,0.006Tb 3+ ,0.05Ge 4+ to that of the state-of-the-art BaFBr(I):Eu 2+ is ≈1.2 and 2.7, respectively. Force induced charge carrier storage phenomena is studied in the Tb 3+ , Bi 3+ , Ga 3+ , or Ge 4+ doped LiTaO 3 . Proof-of-concept compression force distribution sensing and X-ray imaging is demonstrated by using optimized LiTaO 3 :0.005Bi 3+ ,0.006Tb 3+ ,0.05Ga 3+ dispersed in a hard epoxy resin disc and in a silicone gel film. Proof-of-concept color-tailorable ML for anti-counterfeiting is demonstrated by admixing commercial ZnS:Cu + ,Mn 2+ with optimized LiTaO 3 :0.005Bi 3+ ,0.006Tb 3+ ,0.05Ge 4+ in an epoxy resin disc.