AbstractFlexible regulation of bandgap of perovskite nanocrystals (PNCs) is fundamentally critical for desirable optoelectronic functions and applications. Here, regulating chemical composition and emission wavelength of PNCs in glass by a simple heat‐treatment process are reported, which is established to rely on the thermal‐trigger phase separation and ion exchange. The first principle calculations are overall performed to reveal the mechanism of bandgap engineering and optimization of emission performance. The PNCs exhibit excellent stability against thermal, ultraviolet irradiation, and organic molecules. The bandgap of PNCs in the heat‐treated glass can also be re‐modulated by ultrafast laser irradiation. Ultrafast laser direct writing of multi‐color patterns and holographic dynamic displays are achieved, which hold great potential in the application of encryption‐decryption and emissive devices.