The green light-emitting aluminosilicate glass with CsPbBr3 quantum dots (QDs) is prepared by the melt-quenching and heat-treatment method. The effect of perovskite composition modulation on the crystallization of CsPbBr3 QDs in glass matrix is discussed in detail. By optimizing the perovskite composition in the fluorosilicate SiO2–Al2O3–Li2CO3–AlF3–LiF glass system, the photoluminescence quantum yield (PLQY) of QDs glass under 365 nm excitation reaches 26.51%. The obtained CsPbBr3 QD glass shows outstanding uniformity, thermal stability and water resistance. White light-emitting diode (WLED) fabricated by using the green QDs glass powder and red nitride commercial phosphor with blue InGaN chip displays luminous efficiency of 24.68 lm/W with CIE coordinates of (0.3361, 0.3300) and correlated color temperature of 5322 K at 10 mA.