Herein, we first prepared polychromatic self-crystallized CsPb(Cl/Br/I)3 perovskite nanocrystalline (PN) borosilicate glass by the high-temperature melting method. Then, the PN glass is exposed to frequent mechanical ball milling. Due to the high-energy mechanical force, the microstructure changes in borosilicate glass such as topological structure, chemical short-range order, and atomic rearrangement lead to the secondary crystallization of PN on the glass surface. Hence, the photoluminescence quantum yield (PLQY) of CsPbBr3 PN glass has enhanced 120 times and that of CsPbBrI2 PN glass has enhanced 74 times. Moreover, the prepared highly luminescent CsPbBr3 PN glass has extremely large exciton binding energy (468 meV), which shows good thermal stability. Finally, by embedding the prepared PN glass powder in the polydimethylsiloxane matrix, multicolor luminescent flexible films are constructed, presenting application prospects in the flexible display field. This work deepens the understanding of how the microstructure change in glass influences the crystallization behavior of PN and resolves the challenge that PN glass cannot have high PLQY and stability at the same time.