Carbanion-based ionic liquids are proposed and utilized as the key components for the construction of five super-nucleophilic deep eutectic solvents (SNDESs) in the paper. The super-nucleophilic nature of carbanion-based ILs is found to enable the capture of CO₂ with large absorption capacity. However, the absorption is very slow in the IL due to high viscosity. The synergy of carbanion siting and hydrogen bonding is found to enable high and fast absorption of CO₂ in [N₂₂₂₂][CH(CN)₂]-ethylimidazole (Eim), and a synergistic absorption mechanism is proposed and validated from spectroscopic analyses and quantum calculations. The enthalpy change of CO₂ absorption in [N₂₂₂₂][CH(CN)₂]-Eim is calculated to be -39.6 kJ/mol according to the thermodynamic model, and the moderate value implies that both absorption and desorption of CO₂ in the DES are favored and well balanced. The synergism of carbanion and hydrogen bond mediated by SNDESs provides a novel insight into the efficient CO₂ capture.