Aluminum (Al)–aluminum–carbon nanotube (Al–CNT) dual-matrix (DM) composites are a novel class of nanocomposite materials that combine the ductility of the Al matrix with the hardness and wear resistance of the Al–CNT composite and thus can offer a unique combination of properties that make them suitable for a wide range of wear applications such as cutting tools, bearings, brake pads, wear-resistant coatings, etc. However, the specific properties of the DM Al–(Al–CNT) composite will depend on several factors related to the material’s composition and the friction conditions. This study investigates the wear behavior of DM Al–(Al–CNT) composites consisting of a primary matrix of soft aluminum in which milled hard particles of (Al–CNT) are dispersed as affected by five parameters: (1) wt.% CNT in the reinforcement particles, (2) mixing ratio between the reinforcement particles and the soft Al matrix, (3) sliding speed, (4) applied load, and (5) distance. The experimental design used a Taguchi fractional factorial orthogonal array (OA) L27 to reduce the number of experiments, and analysis of variance (ANOVA) was used to determine the significance and to model the effect of each control parameter. Results showed that the wear rate could be reduced by up to 80% by tailoring the composition and controlling the friction conditions. It was found that the mixing ratio significantly impacts the wear behavior of DM Al–(Al–CNT) composites. A mixing ratio of 50% and a CNT content of 3 wt.% at the lowest applied load gave the lowest wear rate and coefficient of friction. Scanning electron microscopy investigations showed fragmentations in the reinforced matrix at higher loads and mixing ratios, which negatively impacted the wear behavior. Our findings confirm that DM Al–(Al–CNT) composites are promising for wear applications. However, the wear behavior depends on the composition and microstructural design of the composite, which needs to be carefully studied and understood.