This paper proposes for the first time the preparation of a series of amino acid ionic liquids (AAILs) via one-step hydrolysis of cheap lactams for the capture of CO2. The structures of the prepared AAILs are confirmed using NMR, FTIR, and ESIMS, and their physical properties are also determined. It is found that these AAILs are reversible CO2 absorbents with very high absorption capacities (0.15 to 0.18 g·g1 at 313.2 K and 1.0 bar), better than almost all task-specific ionic liquids reported in literatures. The absorption mechanism is also elucidated to be a combination of 1:1 and 2:1 stoichiometric reaction of AAILs with CO2 from NMR, FTIR, reaction equilibrium thermodynamical modelling (RETM) and quantum calculations. The AAILs have the advantages of simple synthesis, high yield, and using available cheap raw materials. It is believed that this kind of AAILs have great potentials to be used as efficient CO2 absorbents.