The study explores the microstructural design of hybrid Al2O3–Cu–Me composites formed by centrifugal slip casting into porous molds. Obtained composites are characterized by zones with different contents of metal phases. It was determined that there are two mechanisms driving thickening of slurries: capillary forces influencing smaller particles and centrifugal forces affecting larger particles. To enhance composite’s cracking toughness, a gradient distribution of metallic phase with highest metal concentration near surface is essential. This is achieved by optimizing ceramic powder size, limiting processing time, and using gel centrifugal casting to eliminate undesired zones. Zone II’s width is influenced by metallic phase proportion, mold rotation speed, and compaction rate, with heavier particles and greater metal content near outer surface. Zone III expands with lower rotational speeds and lighter metallic particles. The mutual reactivity and solubility of selected metallic elements also play a crucial role in the final microstructure. The findings highlight the potential for precise control over composite microstructures through careful selection of metallic elements, powder sizes, and casting parameters, offering valuable insights for model research and simulations.