Advances in reactive CO2 capture and mineralization for delivering carbon management solutions and co-producing carbonate materials for use in construction materials provide unique opportunities to advance the efficiency of heavy industries. In reactive CO2 capture and mineralization, CO2 is captured using amines and amino acids, and the resulting CO2 loaded solvents are directly reacted with alkaline residues to co-produce solid carbonates while regenerating the solvents. Unlike conventional CO2 capture or mineralization alone, the availability of basicity from the solvents and the solid residues in reactive CO2 capture and mineralization accelerates CO2 uptake. In this work, detailed laboratory-scale experiments of reactive CO2 capture and mineralization are complemented with NMR investigations of the solvents to investigate the underlying molecular-scale mechanism and develop a strategy towards scale-up. Multifunctional solvents that enable selective uptake of CO2, limit SOx and NOx uptake, and enable ease of carbon mineralization, can be effectively regenerated via carbon mineralization; and can be reused over multiple cycles of operation are also identified through this effort. To summarize, this effort unlocks the mechanistic basis for choosing multifunctional solvents for reactive CO2 capture and solvents and enables scale-up of the technology to meet industrial needs.