Overcoming inherent brittleness and poor crack resistance (CR) of inorganic glasses is crucial to widen their applications. By optimizing the thermal treatment scenarios, a transparent surface crystallized aluminosilicate glass with an ultrahigh CR (75.1 N) and high hardness (7.1 GPa) is fabricated. Compared with the as-prepared glass with the stoichiometric β-quartz s.s. composition (Li2O·Al2O3·2.5SiO2), a near 14 times enhancement in CR is exhibited, which could be one of the reported glasses with the highest CR. The evolution of phase compositions and morphologies with modifying thermal treatment protocols was revealed through characterization. And the processing parameter dependence behaviors of mechanical performances for these crystallized glasses is mainly ascribed to the alterations in grain size, preferred orientation, or fraction of β-spodumene s.s. and β-quartz s.s. crystal phases in the surface crystallized layer. These findings provide new insights for developing new transparent materials with ultrahigh crack resistance to fulfill the applications such as electronic screens.