This research work investigates the root causes of wear on the tribo surface of mechanically alloyed Aluminum/CNT composite through a simulated in situ analysis. The wear maps are developed using the second-order polynomial regression equation for the Aluminum/CNT composite to discriminate the wear mechanisms at different levels of their influencing factors and milling parameters. As a result, the predominant wear mechanism is identified as surface fatigue for Aluminum/CNT composite under high loading dry sliding condition. This study also reveals the modes for eliminating the severe wear at the tribo-surfaces. Aluminum/CNT1 wt% composite fabricated with the mechanical alloying parameters above 6 h of milling time and above 5 rps of milling speed eliminates the delamination under low level of tribological parameters, and it achieves the minimal wear-rate of 30.5 × 10−6 g/m and coefficient of friction (CoF) of 0.346.