We manipulated soft coarse-grained (CG) domains to design optimized and toughened B4Cp/6061Al composites, featuring bimodal domains with in-situ MgO nanoparticles (n-MgO) and ex-situ carbon nanotubes (CNTs). Manipulating CG fractions influenced heterostructure parameters such as CG band width and domain distribution. A systematic optimization strategy integrating intrinsic/extrinsic toughening and strengthening mechanisms identified optimal conditions for maximizing strength-ductility-toughness. The optimal 20:80 CG-to-ultrafine-grain (UFG) weight ratio offered an ultimate strength of 550 MPa and ∼7 % elongation. Intrinsic toughening mechanisms enhanced UFG domain dislocation storage capacity. Multiscale analysis of crack behavior revealed pronounced crack-blunting in well-dispersed CG domains. Extrinsic toughening mechanisms included nanobridge formation, crack-deflection, micro-crack proliferation, and crack-branching. Micromechanical behavior was examined using the strain gradient model. Designing strong and ductile micro/nano-reinforced bimodal grained composites requires selecting a smaller amount of CG domains, a CG band width larger than double the interface affected zone (IAZ), and larger grain sizes in the CG domains.
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