In carbon nanotube (CNT) reinforced metal-matrix composites, a strong interface between CNTs and the matrix is essential for an effective load transfer. Otherwise, the excellent qualities of CNTs would virtually remain unexploited. The aim of this study is to investigate the effect of Al4C3 formation on the mechanical properties of CNT/Al composites. Composite powders were produced through a three-stage process; First, CNTs were sufficiently crushed via high-energy milling of 20 h. Then, the crushed CNTs were ultrasonically mixed with raw CNTs (in an ethanol medium) followed by a wet milling process. Finally, different amounts of the obtained reinforcing agent (0.5, 1, 1.5, 2, and 3 wt.%) were milled with aluminum powders. Composite powders were subsequently consolidated using spark plasma sintering (SPS) process at two different temperatures (500 and 550 °C) For each sample, the amount of carbide was calculated in a semi-quantitative manner using Raman spectroscopy. The results of phase analysis and mechanical-behavior evaluations showed that Al4C3 formation, due to the consumption of highly-activated crushed CNTs, could improve the interface bonding state while maintaining CNTs structural integrity. Moreover, mechanical and wear tests revealed that the optimum properties were obtained for the composite reinforced by 1wt.% processed carbon nanotubes (PCNTs) and SPSed at 550 °C for 10 min. These findings can open up a window toward the realm of design and processing of CNT/Al composites.