Enhancing the strength and toughness of aluminum alloys using microstructure optimization remains a key challenge. In this study, an AA2024 aluminum alloy with a double-layer multi-gradient structure was fabricated using 50% constrained deformation and single-stage peak aging at 150 °C. Microstructural and compositional analysis was performed using SEM, XRD, and TEM to investigate grain structures, dislocation density, and the distribution of precipitated phases. The results revealed a heterogeneous microstructure with variations in grain size, dislocation gradient, and precipitation phases between the constrained and deformation layers. Mechanical testing demonstrated a 30.9% increase in yield strength, a 16.4% increase in tensile strength, and a 13.9% improvement in uniform elongation compared to the T6 temper. Corrosion tests showed enhanced resistance, with a shallower intergranular corrosion depth and higher self-corrosion potential. The improved mechanical properties were attributed to the dislocation gradient and heterogeneous precipitation phases, while the enhanced corrosion resistance resulted from the transformation of the S phase from a continuous grain boundary distribution to a discontinuous distribution along dislocations. This study provides a novel approach for optimizing the mechanical and corrosion properties of AA2024 aluminum alloy using microstructure design and precise thermal–mechanical treatment.