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The 2024Al matrix composite reinforced with bimodal-scaled reinforcement phases, carbon fibers and ZrC particles, was designed and prepared by spark plasma sintering for the purpose of obtaining high strength and good ductility. The microstructural observation shows that the ZrC particles mixed with the Al2Cu and Al2CuMg precipitate phases formed a quasi-network architecture. The Ni coating electroless plated on the carbon fiber can improve the interfacial bonding strength by the chemical reactions of Ni-P coating and matrix as well as prevent the reaction of carbon fiber and 2024Al. As expected, the tensile strength and ductility of bimodal-size reinforced composites with peculiar quasi-network structure showed a significant improvement in comparison with the 2024Al matrix alloy and monolithic carbon fibers or ZrC particles reinforced composites. The 2024Al matrix composites strengthened with carbon fibers and ZrC particles exhibit the tensile strength and elongation of 330 MPa and 10.2%, which are 39.2% and 229% higher than the 2024Al matrix. The excellent enhancement effect is owing to load transfer effect, quasi-network structure strengthening, precipitation refinement, Orowan strengthening as well as dislocation strengthening.