Ionic liquids (ILs) are eco-friendly solvents and exhibit excellent performance for dissolution and regeneration of wool keratin. In this work, a series of ILs are designed and synthesized to investigate effects of ILs structures on dissolving wool keratin and properties of regenerated keratin. The results show that both cations and anions have important impacts on dissolution capability for wool, while side chain lengths of imidazole cation have little effect. Structures and properties of regenerated keratin are characterized by various techniques such as FT-IR, NMR, SEM, TGA and XRD. It is found that the dissolution time is shorten to 1.5 h by[Emim]DMP, thermal stability of regenerated keratin from its solution is superior to that from Bmim]OAc solution, and the proportion of α-helix structure is as high as 78.7%. In addition, five cycles of [Emim]DMP suggest that it has a good reusability, and the rheological property of DPILs solutions shows their excellent potential for fiber spinning.