AbstractGraft copolymerization of vinyl monomers, mainly methyl methacrylate, in reduced, successively alkylated, or KCN‐Treated wool fibers was performed in the redox LiBr–persulfate system without homopolymer. The reduction gives a striking effect in promoting the graft copolymerization. Methylation or ethylene recrosslinking of the reduced wool, especially the former, decreases the graft‐on remarkably. By the KCN treatment in which the conversion of disulfide to lanthionine bonds occurs, the grafting is decreased in the bromide–persulfate system but promoted in the system with persulfate alone. Methylation or KCN treatment of wool as well as reduction brings about a great increase in the absorption of persulfate. The grafting of the lanthionine‐containing wool in the redox system accompanied by the liberation of bromine might be retarded by the pronounced bromination of monomers over the inhibiting of homopolymerization, because the lanthionine bonds are more stable to bromine than the disulfide bonds. In general, disulfide bonds and the other easily oxidized components of wool may perhaps play an important role in regulating the bromination of monomers and in the graft copolymerization without homopolymer. The molecular weight of graft polymer is decreased distinctly with increasing extent of reduction of wool. From these results, the thiol groups on wool are considered to give predominantly graft centers by the radicalotropy from SO4 −·, O
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