In this study, we present a computational thermodynamic strategy to obtain a minor but optimum amount of additional element into a base alloy to improve its glass-forming ability, through thermodynamically calculating the maximum liquidus depressions caused by various alloying addition ͑or replacement͒ schemes. We demonstrate the successful use of Zr 56.2 Cu 31.3 Ni 4.0 Al 8.5 as the base alloy with the addition of 4.9% Ti, by observing a significant increase in the glass-forming ability of more than 100% in terms of the diameter of the glass formed from the base alloy to the one with the addition of 4.9% Ti. The approach presented here can be considered as a universal method to synthesize novel and bulkier metallic glasses not only of scientific interest but also potential technological applications. , respectively. This success has provided a fresh impetus to the idea that micro-or minor alloying represents an effective way to develop novel bulkier metallic glasses. However, due to the complex nature of the multicomponent interactions involved, the underlying mechanism upon the enhancement of glass-forming ability ͑GFA͒ by minor alloying still remains a puzzling mystery. It thus becomes difficult to identify the optimum amount of a potential element, a priori, for improving the GFA of a known glass-forming alloy. Neither the recent compelling structural model proposed by Miracle, 3 nor current atomistic simulation, such as reverse Monte Carlo and molecular dynamics simulation, is able to make such predictions. 4,5 Here, using Al-Cu-Ni-Zr-Ti as a model system, we present a robust computational thermodynamic approach to obtain multicomponent phase diagrams; 6 on the basis of which, we are able to formulate a practically useful strategy for pinpointing bulkier glass-forming compositions of Al-Cu-Ni-Zr with optimum Ti-alloying additions.A strong indication drawn from the aforementioned experimental works 1,2 is that the Y-enhanced GFA of the Cuand Fe-based alloys is accompanied by a substantial depression in the liquidus temperature caused by the addition of Y, and the bulkiest Y-alloyed BMGs are those possessing the deepest liquidus depressions compared with the base alloys. These findings are in accord with the known GFA criteria, such as T rg ͑=T g / T l , where T g is the glass transition temperature and T l is the liquidus temperature͒ andwhere T x is the temperature of the onset of crystallization͒, both of which indicate that decreasing the liquidus temperature facilitates easier glass formation. 7,8 In thermodynamics, the existence of an alloy liquid toward lower temperatures is a manifestation of its increasing thermodynamic stability when compared with its competing crystalline phases as the temperature is lowered. Although this is a necessary but not a sufficient condition, decreasing temperature increases the liquid's viscosity ͑with corresponding decreases in its diffusivity͒.9 This in turn, kinetically, also favors glass formation. Thus, in this letter, we use the liquidus temperature ͑or depression͒...