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As a promising architecture reinforcement, the three-dimensional (3D) configuration of nanocarbon holds great prospects in achieving a strength-ductility combination for metal matrix composite (MMCs). However, due to the native deficiency of Al in catalyzing the growth of nanocarbon, constructing a nanocarbon network has been the long-term challenge for Al matrix composites (AMCs). Herein, we develop a new strategy for synthesizing AMCs reinforced by three-dimensional nanocarbon (3D-C) via plasma-enhanced chemical vapor deposition (PECVD) integrated with hot pressing (HP) as well as hot extrusion, demonstrating exceptional mechanical properties. The detailed characterization reveals that the in-situ generation of nanocarbon layers on the surface of Al powders is attributed to the initiation of isolated carbon islands, followed by merging and self-assembly, which is governed by the PECVD-assisted …