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Wool is a natural biopolymer with excellent biocompatibility. This dense structure makes it difficult to recycle the millions of wool textiles discarded annually. This study reports, for the first time, the regeneration of keratin using thiourea dioxide. Disulfide bonds were cleavage from the result of Raman test. FTIR, XRD and 13C-NMR tests determined that regenerated wool keratin retained protein macromolecule backbone, though the crystallinity degree and α-helix structure content decreased slightly. SDS-PAGE results demonstrated that the process contributed to an increase of low molecular weight keratin. All the results in this study indicate that thiourea dioxide is an effective solvent for the regeneration of wool keratin. The study offers a novel approach for the regeneration and recycle of other natural protein-based material. [ABSTRACT FROM AUTHOR]