A series of Al25 − xCr25 + 0.5xFe25Ni25 + 0.5x (x = 19, 17, 15 at%) multi‐component alloys are prepared by arc‐melting and rapid solidification of copper molds. The technique of thermal‐mechanical processing is further applied to the master alloys to improve their mechanical properties. These alloys consist of face‐centered cubic (FCC) and body‐centered cubic (BCC) structure. The volume fraction of the BCC phase increases as Al content increase and Cr and Ni contents decrease, accompanied with a microstructural evolution from dendritic structure to lamella‐like structure. Due to the increase of volume fraction of BCC phase, the master alloys exhibit an increased strength and a declined ductility as Al content increases. The rapid solidified alloys have more BCC phase compared with the master alloys, which enhances the strength and decreases the ductility. After homogenization, hot‐rolling, and annealing at 1000 °C, the Al8Cr33.5Fe25Ni33.5 alloy displays excellent combination of strength (yield strength is ∼635 MPa and fracture strength is ∼1155 MPa) and ductility (tension strain is ∼11%).