LAUSR

The antagonism between strength and corrosion resistance in graphene‐reinforced aluminum matrix composites is an inherent challenge to designing reliable structural components. Heteroatom microstructural modification is highly appreciated to conquer the obstacle. Here, a bottom‐up strategy to exploit the heterogeneous phase interface to enable high corrosion durability is proposed. Deformation‐driven metallurgy derived from severe plastic deformation is developed to produce Mg‐alloyed fluorinated graphene structures with homogeneous dispersion. These structures allow for absorbing corrosion products, forming a dense protective layer against corrosion, and local micro‐tuning of the suppression of charge transfer. This results in superior corrosion resistance with an outstanding strength‐ductility balance of the composites via ultrafine‐grained and precipitation strengthening. The anti‐corrosion polarization resistance remains 89% of the initial state after 2‐month immersion in chloride‐containing environment, while the ultra‐tensile strength and elongation of 532 ± 39 MPa and 17.3 ± 1.2% are obtained. The economical strategy of heteroatom modification broadens the horizon for anti‐corrosion engineering in aluminum matrix composites, which is critical for the design of carbonaceous nanomaterial‐reinforced composites to realize desired performances for practical applications.