Limestone (calcite) calcined clay cement (LC3) is a promising low-CO2 binder, but the low activity of calcite cannot compensate the reduction in clinker factor, resulting in low one-day strength and limiting its broad applications. As recent carbon capture and utilization technologies allow scalable production of vaterite, a more reactive CaCO3 polymorph, we overcome the challenge by introducing vaterite calcined clay cement (VC3), inspired by the vaterite-calcite phase change. In the present study, VC3 exhibits higher compressive strengths and faster hydration than LC3. Compared to hydrated LC3, hydrated VC3 exhibits increased amount of hemi- and mono-carboaluminate formation and decreased amount of strätlingite formation. With gypsum adjustment, the 1-day strength of VC3 is higher than that of pure cement reference. VC3, a low-CO2 binder, presents great potential as a host of the metastable CaCO3 for carbon storage and utilization and as an enabler of carbon capture at gigaton scales.