The rising atmospheric CO2 concentration reaching nearly 40 billion tonnes every year has prompted widespread global concern about greenhouse gas (GHG) emissions leading to severe global warming. Carbon-sequestered concrete (CSC) emerges as a promising solution for addressing climate change through utilising CO2 on a significant scale, fostering a sustainable future in the construction industry. Further, integrating green binders such as Ground Granulated Blast Furnace Slag (GGBFS) into conventional concrete could mitigate a substantial portion of approximately 4 billion tonnes of global CO2 emissions annually arising from the calcination processes in cement manufacturing industries. With the aim of harnessing this capacity, the authors attempted to evaluate and enhance the carbon sequestration of GGBFS-added concrete and cement binder types, using a state-of-the-art CO2 mixing and CO2 curing facility. Various investigations were performed to understand its influence on CO2 Uptake Capacity, Strength and Microstructure. This sustainable concrete-producing technology demonstrated a momentous overall CO2 Uptake of 20.04% (which included an enhanced CO2 uptake of more than 13%), thereby showcasing the potential for realising India’s ambitious goal of achieving carbon neutrality by 2070. Further, it was able to improve the compressive strength by up to 19.90% and reduce pore sizes to <1 mm on account of densification and microstructure enhancement.