SummaryConventionally, high-throughput computational materials searches start from an input set of bulk compounds extracted from material databases, but, in contrast, many real functional materials are heavily engineered mixtures of compounds rather than single bulk compounds. We present a framework and open-source code to automatically construct and analyze possible alloys and solid solutions from a set of existing experimental or calculated ordered compounds, without requiring additional metadata except crystal structure. As a demonstration, we apply this framework to all compounds in the Materials Project to create a new, publicly available database of>600,000 unique “alloy pair” entries that can be used to search for materials with tunable properties. We exemplify this approach by searching for transparent conductors and reveal candidates that might have been excluded in a traditional screening. This work lays a foundation from which materials databases can go beyond stoichiometric compounds and approach a more realistic description of compositionally tunable materials.