In this study, the interactional effects of CNT vol%, milling energy, and temperature on the hardness, tensile strength, and shear strength of Al-CNT composites fabricated through flake powder metallurgy were evaluated experimentally and through MD simulations. The results showed that the CNT content and milling energy significantly influenced the deformation behavior of composite, primarily due to their impact on interfacial bonding strength and dispersion quality. MD simulations were used to study atomistic interactions under loading, including the generation, proliferation, and accumulation of dislocations, slipping of shear planes, and the production of shear bands. These simulations provided insights into the load-bearing mechanisms of CNTs and the nucleation and propagation of dislocations at the interface, which improved the properties of composite. The optimized Al-CNT composite exhibited remarkable properties, with a hardness of 62.8 HB, a tensile strength of 150.7 MPa, and a shear strength of 126.2 MPa, all significantly higher than those of pure aluminum. A confirmatory test demonstrated excellent correlation between experimental and predicted results.