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Concrete 3D printing is a sustainable solution for manufacturing efficient designs and creating less waste, and selecting the optimal materials to use can amplify the advantages of this technology. In this study, we explore printing lightweight concrete by replacing normal weight aggregate with lightweight aggregates such as cenospheres, perlite, and foam beads. We adopt a systematic approach to investigate mixtures using different formulation methods such as the specific gravity and packing factor methods to improve the printing and mechanical performances of the mixtures. The rheological results showed significant improvement in the flow characteristics of the different mixtures using both the specific gravity method and the packing factor method to formulate the mixtures. Furthermore, a statistical tool was used to achieve optimal performance of the mixtures in terms of high specific compressive strength, high flow characteristics, and good shape retention capability by maximizing the specific compressive strength ratio, slump flow, and the static yield stress, while minimizing the slump, dynamic yield stress, and plastic viscosity. With the above design objectives, the optimal percentages of the aggregate replacements (cenosphere, perlite, and EPS foam beads) were 42%, 68%, and 44%, respectively. Finally, the optimized results also showed that the mixture with cenosphere aggregate replacement had the highest specific strength.