The increasing demand for higher performing materials across many fields requires the development of ever more complex materials. In this project a novel materials discovery methodology will be developed based on advances in combinatorial computational thermodynamics and experimental techniques. Bulk metallic glasses will be taken as example materials because of their technological potential - they can be considered high-strength metals that can be formed like plastics - and their suitability for the development of a general methodology. Many alloys - on the order of thousands - will be synthesized and characterized simultaneously. The ability of these alloys to be deformed, a property that correlates with the glass forming ability, will be measured experimentally. The crystalline phases competing with the glassy phase will also be characterized. These crystalline phases will be compared with atomic modeling results considering the energy of many possible crystalline phases. Since direct modeling of the glass forming ability is not possible from first principles, correlations will be established between the experimental glass forming ability and the competing crystalline phases from atomic modeling. The development of such a methodology and correlation through this research will accelerate the pace of discovery and deployment of advanced materials.