Article discusses how, in this study, processing–structure–property relations were systematically investigated at room and elevated temperatures for two FCC Al0.3CoFeCrNi and Al0.3CuFeCrNi2 high-entropy alloys (HEAs), also known as complex concentrated alloys (CCAs), prepared by conventional arc-melting. It was determined that both alloys exhibit FCC single-phase solid solution structure. Micro-indentation and sliding wear tests were performed to study the hardness and tribological behavior and mechanisms at room and elevated temperatures.