This work systematically investigated the effect of dual shot peening (DSP) and conventional shot peening (CSP) on the microstructure, residual stress and wear performance of the CNT/Al-Cu-Mg composites. The results indicated that compared with CSP, DSP effectively reduced surface roughness (Rz) from 31.30 to 12.04 μm. In parallel, DSP introduced a smaller domain size (33.1 nm) and more dislocations, higher levels compressive residual stress and a stiffer deformation layer with deeper affected zones. Moreover, DSP effectively improved the uniformity of the surface layer's microstructure and residual stress distribution. The improvement is mainly due to secondary impact deformation by microshots and fine grain strengthening. In addition, the transformation of the hard second phases such as Al4C3 and CNT and its effects on improving the surface strength and deformation uniformity were discussed. Significantly, DSP improved the wear resistance by 31.8% under the load of 6 N, which is attributed to the synergistic influence of factors including hardness, compressive residual stress, surface roughness, and grain size. In summary, it can be concluded that DSP is an effective strategy to promote the surface layer characteristics for CNT/Al-Cu-Mg composites.