Epitaxial growth of halide perovskite heterostructures endows unique electronic structures for diversified luminescent properties. Herein, an epitaxial growth strategy is proposed to assemble MgGa2O4/CsPbBr3 heterostructure with dynamic photoluminescence. Interface defect passivation during integration transforms interstitial and antisite interface defects of CsPbBr3 nanocrystals to shallow states, enhancing photoluminescence stability of the heterostructure against irradiation, solvents, and heat as well. Finally, the as‐constructed heterostructure shows a reversible dynamic photoluminescence from green to blue under 254 nm ultraviolet (UV) irradiation, which is attributed to the electron injection from shallow defects to the emission centers in MgGa2O4 and CsPbBr3 with different radiative recombination rates. Encryption applying binary encoding method based on MgGa2O4/CsPbBr3 and dynamic anti‐counterfeiting feature of its polymer hybrid film are further investigated.