Bulk metallic glasses (BMGs) exhibit high yield strength but little tensile ductility. For this class of materials, damage tolerance is a key mechanical design parameter needed for their engineering use. Recently we have discovered a correlation between the local structural characteristics in the glass and the propensity for shear transformations. Based on the dependence of glass structure on alloy composition, zirconium (Zr)-rich Zr–titanium (Ti)–copper (Cu)–aluminum (Al) compositions are predicted to be more prone to spread-out plastic deformation and hence profuse shear banding. This structural perspective has guided us to locate a Zr61Ti2Cu25Al12 (ZT1) BMG that exhibits a record-breaking fracture toughness, on par with the palladium (Pd)-based BMG recently developed at Caltech. At the same time, the new BMG consists of common metals and has robust glass-forming ability. Interestingly, the ZT1 BMG derives its high toughness from its high propensity for crack deflection and local loading-mode change (from mode I to substantially mode II) at the crack tip due to extensive shear band interactions. A crack-resistance curve (R-curve) has been obtained following American Society for Testing and Materials (ASTM) standards, employing both “single-specimen” and “multiple-specimen” techniques as well as fatigue precracked specimens. The combination of high strength and fracture toughness places ZT1 atop all engineering metallic alloys in the strength–toughness Ashby diagram, pushing the envelop accessible to a structural material in terms of its damage tolerance.