Aluminum alloys, known for their high strength-to-weight ratios and impressive electrical and thermal conductivities, are extensively used in numerous engineering sectors, such as aerospace, automotive, and construction. Recently, significant efforts have been made to develop novel aluminum alloys specifically tailored for additive manufacturing. These new alloys aim to provide an optimal balance between mechanical properties and thermal/ electrical conductivities. In this study, nine combinatorial samples with various alloy compositions were fabricated using direct energy deposition (DED) additive manufacturing by adjusting the feeding speeds of Al6061 alloy and Al-12Si alloy powders. The effects of the alloying elements on the microstructure, electrical conductivity, and hardness were investigated. Generally, as the Si and Cu contents decreased, electrical conductivity increased and hardness decreased, exhibiting trade-off characteristics. However, electrical conductivity and hardness showed an optimal combination when the Si content was adjusted to below 4.5 wt%, which can sufficiently suppress the grain boundary segregation of the α- Si precipitates, and the Cu content was controlled to induce the formation of Al₂Cu precipitates.