Unlike ordered and stoichiometric compounds, alloys represent a continuous compositional space and structural disorder adds to the complexity. Designing alloys to optimize functional properties in this continuous chemical space while also accounting for the effects of structural disorder is a formidable task. Empirical approaches have been quite successful for alloy design, especially high-throughput combinatorial thin film synthesis techa University of Illinois at Urbana-Champaign, Urbana, IL 61801. b University of Colorado School of Mines, Golden, CO 80401. ⇤ Email: pgorai@mines.edu † Electronic Supplementary Information (ESI) available niques. However, applications such as thermoelectrics that require synthesis of bulk (vs. thin-film) samples, alloy optimization remains a tedious experimental process relying on trial-and-error and chemical intuition.