The modulated structure of the AlCrFeCoNiCu high-entropy alloy consists of NiAl intermetallics (β′) and a (α-Fe, Cr) solid solution (β). The formation of the NiAl intermetallics greatly affects the strengths and magnetic properties of the AlxCrFeCoNiCu alloys. Evidently, the AlCrFeCoNiCu alloy cannot be treated as a solid-solution alloy.