In this work, we demonstrate an innovative strategy for efficient and sustainable absorption of NO in a series of ionic liquids (ILs) containing amine groups and azole groups. The results show that the ILs have low viscosities and high performance for NO absorption. For instance, [TEPA] [Im] had a high absorption capacity of 6.79 mol NO per mol IL at 30 degrees C and ambient pressure. The absorbed NO was easily released by heat treatment, and the regenerated IL had significant reversibility. The results of H-1 NMR, UV spectra, and FT-IR spectra of ILs before and after NO absorption indicated that the absorption of NO in the [TEPA] [Im] mainly resulted from a chemical interaction. NO interacts with not only the secondary amine groups in the cation but also N-imidazole in the anion through the formation of NONOate, indicating [TEPA] [Im] is a dual functional IL. By introducing this efficient and reversible absorption of NO by ILs, our work broadens the method of NO capture.