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In this work, three novel complex concentrated aluminum alloys were developed. To investigate the unexplored region of the multicomponent phase diagrams, thermo-physical parameters and the CALPHAD method were used to understand the phase formation of the Al₈₀Mg₅Sn₅Zn₅Ni₅, Al₈₀Mg₅Sn₅Zn₅Mn₅, and Al₈₀Mg₅Sn₅Zn₅Ti₅ alloys. The ingots of the alloys were manufactured by a gravity permanent mold casting process, avoiding the use of expensive, dangerous, or scarce alloying elements. The microstructural evolution as a function of the variable element (Ni, Mn, or Ti) was studied by means of different microstructural characterization techniques. The hardness and compressive strength of the as-cast alloys at room temperature were studied and correlated with the previously characterized microstructures. All the alloys showed multiphase microstructures with major α-Al dendritic matrix reinforced with secondary phases. In terms of mechanical properties, the developed alloys exhibited a high compression yield strength up to 420 MPa, high compression fracture strength up to 563 MPa, and elongation greater than 12%.