A compositional approach to designing alloys that have an enlarged equiaxed zone is suggested in this study. The partitioning of elements during the solidification of CoCrFeMnNi high-entropy alloy (HEA) was confirmed through a directional solidification quenching experiment. Several HEAs were designed to maximize the effects of constitutional and thermal undercooling by considering factors including solute enrichment at the columnar front and the melting temperatures and thermal conductivities of the individual elements. The newly designed HEAs were shown to have successfully enlarged equiaxed zones, and improved anisotropic properties.