Aluminum alloys are widely utilized in diverse industries, such as automobiles, aerospace, and architecture, owing to their high specific strength and resistance to oxidation. However, to meet the increasing demands of the industry, it is necessary to design new aluminum alloys with excellent properties. Thus, a new method is required to efficiently test additively manufactured aluminum alloys with various compositions within a short period during the alloy design process. In this study, a combinatory approach using a direct energy deposition system for metal 3D printing process with a dual feeder was employed. Two types of aluminum alloy powders, namely Al6061 and Al-12Cu, were utilized for the combinatory test conducted through 3D printing. Twelve types of Al-Si-Cu-Mg alloys were manufactured during this combinatory test, and the relationship between their microstructures and properties was investigated.