This study aimed at understanding the structure and properties of dual-phase eutectics in ternary, quaternary, and quinary alloys of the Al-Co-Cr-Fe-Ni system. The alloys at case were i) Ni₄₈Fe₃₄Al₁₈, ii) Ni₄₄Fe₂₀Cr₂₀Al_16, and iii) Ni_34.4Fe_16.4Co_16.4Cr_16.4Al_16.4. Samples in the form of cylindrical bars, diameter 10 mm × 150 mm, were produced by arc melting and suction casting from pure elements (>99.9 wt%). Bridgman solidification at low growth velocity was used to produce additional samples with large eutectic spacing and lamellae thickness of the two phases body-centered cubic (BCC)-B2 and face-centered cubic (FCC) in order to facilitate phase characterization by energy-dispersive X-ray analysis (scanning electron microscopy/energy-dispersive spectroscopy) and nano-indentation. In agreement with thermodynamic calculations, each of the phases was found to be multi-component and contain all alloying elements in distinct amounts. The mechanical properties of the individual phases were analyzed in relation to their composition using nano-indentation experiments. These measurements revealed some insights into “high-entropy effects” and their contribution to the elastoplastic response to indentation loading. Further analysis focused on as-cast as well as heat-treated samples comprising phase fraction measurements, micro-indentation, and miniature testing in three-point bending configuration. For optimum heat treatment conditions, a good balance of strength and ductility was obtained for each of the investigated alloys. Further work is necessary in order to assess their capability as structural materials.