 High-entropy alloys, HEAs, have attracted significant attention due to their unique properties such as strength, ductility and resistance to corrosion. However, discovering new single-phase HEAs has proven difficult due to a lack of an effective strategy for alloy design. Abinicio molecular dynamic simulations were used to identify potential single-phase HEAs and phase diagram calculations were combined with these simulations to further narrow down the search. Three new single-phase HEAs were discovered, FCC alloys of Co-Pham NNI, CUNIPD point, and CUNIPD point RH, and HCP alloys of Co-OS Riru. This article was authored by David E. Ellman and Michael C. Gao.