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Evading the strength-ductility trade-off is essential for engineering application of metal matrix composites. Herein, we propose a novel strategy to achieve the prominent strength-ductility combination of nanocarbon-Al composites. The strategy makes use of the nanocarbon architecture design via longitudinally unfolding the multi-walled carbon nanotubes (CNTs) into graphene nanoribbons (GNRs). It was found that the nano-sized intragranular and interfacial Al₄C₃ (length: 64±23 nm) easily formed in GNR/Al via the “heterogeneous nucleation-growth” pattern, which is contrary to the submicron-sized epitaxial Al₄C₃ (length: 133±39 nm) in CNT/Al. Detailed characterizations reveal the specific orientation relationships between Al₄C₃ and Al in GNR/Al, which benefits the robust interfacial bonding. The intragranular Al₄C₃ and intergranular GNR with large aspect ratio effectively increase the dislocation storage and …