Heterogeneous metallic structures constitute a novel class of materials with excellent mechanical properties. However, the existing process for obtaining heterostructures from a single material does not meet large-scale industrial requirements. In this study, a pure copper heterostructured laminate (HSL) composed of a surface elongated-grain layer and a central equiaxed-grain layer was fabricated by rolling bonding and annealing. To study the effect of the interface on the mechanical properties of gradient-structured materials, both laminate metal composite (LMC) and non-composite laminate (NCL) were fabricated by cold-rolling pretreatment of the center layer (60% reduction) and cold-rolling bonding of the whole blank (67% reduction). Then, the HSL was obtained by controlling the post-annealing regimes, the microstructure of each layer was optimized, and a larger degree of microstructural heterogeneities, such as grain size, misorientation angle, and grain orientation, was obtained, which resulted in obvious mechanical differences. Tensile tests of the HSL, surface layer, center layer, and NCL specimens revealed that the HSL annealed at 300 °C for 1 h had a significantly higher strength than the center layer and a higher elongation than the surface layer. The HSL had a tensile strength and elongation at fracture of 278.08 MPa and 46.2%, respectively, indicating a good balance of strength and plasticity. The improved properties were primarily attributed to the strengthening or strain hardening due to the inhomogeneous deformation of the heterogeneous layers in the laminate and the mutual constraint acquired by the distinct layers with strong mechanical differences. The HSL had an interfacial bonding strength of 178.5 MPa, which played a vital role in the coordinated deformation of the heterogeneous layers. This study proposes an HSL design method that effectively simplifies the process of obtaining heterostructures in homogeneous materials by controlling the cumulative deformation of the surface and center layers.
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