Climate change, driven by rising CO2 levels, is a critical global challenge. Portland cement production, exceeding 4 Gt/year with demand projected to rise by 50%, significantly contributes to this issue. Consequently, there's growing interest in developing low-carbon cementitious binders to reduce the construction industry's environmental impact. This study explores vaterite, a metastable calcium carbonate polymorph, for its potential to enhance cementitious materials' sustainability and performance. Vaterite Calcined Clay Cement (VC3) is investigated as a lowCO2 alternative to traditional cement. Vaterite can sequester approximately 0.44 kg CO2 per kg produced and potentially has a lower manufacturing carbon footprint. Recent advancements have made large-scale vaterite production economically viable, contributing to significant CO2 emission reductions. A scalable vaterite production method was applied utilizing a rapid precipitation technique involving mixing at a 2:1:1 molar ratio of K2CO3, CaCl2, and NH4Cl solutions, followed by filtration and ethanol treatment. This method yields high-purity vaterite making it well-suited for cement applications. The study investigated the effects of varying vaterite content, cement reduction levels, and Metakaolin-to-Vaterite (MK/V) ratios on the compressive strength, and fresh state characteristics of VC3 formulations. Results demonstrated an enhancement of long-term compressive strength (ca. 60% to 80%) of OPC mortar at 28 days when replacing calcite with vaterite up to 15%. Reduction in cement content to 45% and 40% of the total binder proportion, resulted in average compressive strength decreases of 17% and 23%, respectively. Furthermore, results demonstrated that by decreasing MK/V ratio from 3 to 1, compressive strength increases from 20MPa to ca. 27 MPa, that indicates potential pathways for more sustainable formulations. Rheological analysis demonstrated that vaterite improves flowability about 5% compared to calcite, addressing a challenging aspect of traditional Limestone Calcined Clay Cement (LC3) systems. By increasing MK/V ratios from 1 to 3 a decrease in workability of ca. 6% is observed. The effectiveness of polycarboxylate ether (PCE) superplasticizer in enhancing rheology was confirmed across various mix designs. This comprehensive approach to VC3 optimization offers promising pathways for developing high-performance, low-carbon cementitious materials, contributing to the sustainable future of the construction industry and potentially enabling carbon capture at gigaton scales.