This study describes the preparation of bimodal reinforced Cu/Ti3SiC2/C laminated-like composites using flake powder metallurgy and vacuum hot-press sintering process. The objective was to accurately modulate the formation of oriented reinforcement network in two-dimensional carbon materials. The powders used in the five designed composites were flake Cu powder (45–60 μm), Ti3SiC2 (1–5 μm), graphite flakes (GFs, 120 μm) and graphene nanoplatelets (GNPs, 15 μm). Among them, the proportions of Ti3SiC2 (10 wt %) and GFs (3 wt %) remained unchanged, GNPs accounted for 0 wt %, 0.5 wt %, 1.0 wt %, and 1.5 wt %, and Cu powder accounted for a decreasing proportion. Formation mechanisms of GFs and GNPs in oriented networks were quantitatively analyzed using the alignment model. Additionally, the related strengthening and failure mechanisms were investigated. According to the study, the bimodal laminated-like Cu/Ti3SiC2/C composites with 0.5 wt% GNPs added showed the best overall performance. Specifically, it exhibited a hardness of 125.7 HV, tensile strength of 276.3 MPa, thermal conductivity of 207.8 W m−1 K−1, and electrical conductivity of 23.6 MS/m. The network enhanced by the two-dimensional carbon material achieves efficient and orderly load transfer and dissipation mechanisms, optimizing stress distribution and enhancing fracture resistance, resulting in improved mechanical properties. In addition, the formation of the oriented reinforcement network optimizes the orientation arrangement of the reinforcing particles, which somewhat mitigates the scattering of thermoelectric carriers by structural defects in the composites, and the enlarged mean free-range improves the migration efficiency of electrons and phonons. Therefore, the erection of bimodal laminated-like structure achieves the goal of optimizing the properties of the composites.
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