Lightweight Al-based entropy alloys are newly emerged materials with promising potential for structural applications; however, their modeling and strengthening prediction require further exploration. In this study, the spatial distributions of various phases in three Al-based entropy alloys were investigated. A closely interconnected intermetallic compound (IC) network comprising Al2Cu and Al45Cr7 phases was identified. Finite element (FE) modeling was conducted based on the reconstructed three-dimensional microstructure to simulate compressive deformation behavior. The IC network served as the main stress bearer during deformation. Thin sections in the Al2Cu network were the weak sites where stress concentration and damage first occurred. However, the breakage of this limited region contributes to relatively coordinated deformation and extended plasticity. The breakage of large particles accounts for the final alloy failure. The results of the FE model were compared with the experimentally measured stress–strain behavior and mechanical properties, showing very good agreement. Given the non-uniform distribution of strain and stress during deformation, a strengthening model, merging the Voigt and Reuss models, was also developed to predict the mechanical properties of Al-based entropy alloys with the aim of facilitating Al-based entropy alloy development.
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