3D concrete printing (3DCP) has inspired a new generation of architectural and structural designs that combine research advancements in sustainable cementitious materials and material optimized structural geometries. The construction of bio-inspired structural geometry with high specific strength (strength to weight ratio) is now feasible because of the ability of 3D-printing to build intricate and mass-customizable geometries. The 3D printed structures created for this study take inspiration from nature by utilizing geometric shapes of strength and cellular aggregation techniques to create bio-inspired high-performance structures. Taking full advantage of the robotic 3D printing process, such structures can be efficiently customized to reduce material usage for specific load cases in individual structural elements. Beside the reduction of the materials used for construction, the carbon footprint of 3D-printed bio-inspired structures can be further reduced by developing a sustainable-printable concrete. In this study, Portland Limestone Cement (PLC) is used as the base cementitious material for developing the 3D-printable mix. In addition, high dosages of supplementary cementitious materials (SCMs) were used to achieve a high-performance sustainable concrete (HPSC) mixture. The experimental investigation showed that combining bio-inspired structural geometries with HPSC resulted in low-carbon footprint structures with sufficient strength for structural applications.