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This study develops a modified limestone calcined clay cement (LC3) composite for 3D printing, by introducing silica fume (SF) and particle packing theory. Interactions between particle packing density, rheological properties, and printability of the composites were synergistically investigated. Moreover, the ratio of the sand-to-binder (S/B) was also analyzed to explore the performance response. Results show that when composites contain 33.33 wt% calcined clay, 16.67 wt% limestone powder and 5 wt% SF with S/B ratio of 2.5, the dynamic yield stress, static yield stress, and structural recovery can be significantly improved. The proposed mortar can be continuously extruded with few defects and exhibited an excellent shape retention during printing process. Furthermore, the embodied energy (EE) and embodied carbon emissions (ECO₂e) per cubic meter of optimal mortar respectively decreased by 50.2% and 45 …