The major drawback of the aqueous alkanolamine-based carbon dioxide capture process is the high energy penalty for the regeneration of the absorbent. To overcome this weakness, we studied the absorption of CO2 in alkanolamines dissolved in greener and nontoxic deep eutectic solvents. Among the alkanolamines in various deep eutectic solvent media, 2-amino-2-methyl-1-propanol in choline chloride: urea (1:2) medium was found to exhibit the highest absorption capacity for CO2 gas. In addition to that, the value-added product, 2-amino-2-methyl-1-propanol carbamate, was obtained from all deep eutectic solvent medium, which was analyzed by Fourier transform infrared and H-1 and 13C nuclear magnetic resonance spectroscopic techniques. Under optimized conditions, the maximum yield of 82%, 2-amino-2-methyl-1-propanol carbamate was obtained. The deep eutectic solvent used for the process has been recovered and reused for 4 cycles. Thus, the 2-amino-2-methyl-1-propanol in deep eutectic solvent medium emerges to be a novel promising candidate for capture as well as for the utilization of the CO2 gas to obtain the value-added product.