This study investigates the new surface development on AA6061 and AA5086 alloys considering the wire-arc additive manufacturing technique as a direct energy deposition (DED) process of wire. Two different quantities of MWCNTs, i.e., 0.01 (low) and 0.02 (high) g, with a constant nickel (Ni) weight (0.2 g) were pre-placed in the created square patterns. ER4043 filler was used as a wire for additive deposition, and an arc was generated through a tungsten inert gas (TIG) welding source. Furthermore, hardness and pin-on-disk wear-testing methods were employed to measure the changes at the surfaces with the abovementioned inducements. This work was designed to illustrate the hardness and the offered wear resistance in terms of mass loss of the AA6061 and AA5086 aluminum alloys with the function of nano-inducements. Two sliding distance values of 500 m and 600 m were selected for the wear analysis of mass loss from tracks. A maximum increase in hardness for AA6061 and AA5086 alloys was observed in the experiments, with average values of 70.76 HRB and 74.86 HRB, respectively, at a high mass content of MWCNTs. Moreover, the tribological performance of the modified surfaces improved with the addition of MWCNTs with Ni particles in a broader sense; the modified surfaces performed exceptionally well for AA5086 compared to AA6061 with 0.02 and 0.01 g additions, respectively. The system reported a maximum of 38.46% improvement in mass loss for the AA5086 alloy with 0.02 g of MWCNTs. Moreover, the morphological analysis of the developed wear tracks and the mechanism involved was carried out using scanning electron microscope (SEM) images.