<p>Gradient-structured materials have attracted significant attention in metallic structural applications due to their exceptional combination of strength and ductility. In this study, an intermetallic particle-reinforced gradient-structured material (Al₂Cu/Al) was successfully fabricated via twin-roll casting (TRC) process. The eutectic phases, primarily Al₂Cu, were concentrated in the near-surface region of the strip, a result of inverse segregation. To mitigate the aggregation of Al₂Cu eutectic particles, trace amounts of TiC nanoparticles were introduced during the TRC process. The formation of a gradient structure notably enhanced the material’s tensile strength, which can be attributed to two main factors: the load transfer effect of the particles and the back-stress strengthening induced by the gradient in microstructure. This work presents a feasible strategy for the development of high-performance alloys with precisely controlled microstructures, demonstrating the potential of the TRC process for tailoring material properties.</p>