Abstract All‐inorganic CsPbBr 3 perovskite nanocrystals (NCs) have stimulated the enthusiasm of the research on light emitting diodes (LEDs), laser, X‐ray detection, and information encryption, thanks to their excellent optical performance. Exploiting CsPbBr 3 NCs with fascinating long persistent luminescence (LPL) is significantly important for expanding their potential applications. In this work, the room temperature LPL is successfully achieved in CsPbBr 3 glass‐ceramics (GCs) through the optical write with a femtosecond (fs) laser. The carriers captured by the generated trapping centers for the crack of non‐bridged oxygen bonds in the glassy matrix are released by the thermal disturbance of room temperature. Moreover, the LPL performance is modulated flexibly for doping with La 3+ , Dy 3+ , Nd 3+ , and Lu 3+ ions in the CsPbBr 3 GCs, endowing the successful construction of a time‐resolved anti‐counterfeiting mode. Furthermore, the high stability and high color purity (97.04%) of the as‐obtained CsPbBr 3 GCs are demonstrated. The results open a window for fs laser induced perovskite with myriad applications in optical storage devices.