In this study, new high-entropy alloys (HEAs), which contain lightweight elements, namely Al and Ti, have been designed for intermediate temperature applications. Cr, Mo, and V were selected as the elements for the Al-Ti-containing HEAs by elemental screening using their binary phase diagrams. AlCrMoTi and AlCrMoTiV HEAs are confirmed as solid solutions with minor ordered B2 phases and have superb specific hardness when compared to that of commercial alloys. The present work demonstrates the desirable possibility for substitution of traditional materials that are applied at intermediate temperature to Al-Ti-containing lightweight HEAs.