Abstract: The complex hydrogen bond network in wool was deconstructed using the coordination mechanism of lithium ions and bromine ions in a lithium bromide (LiBr) type of deep eutectic solvent (DES). Six different deep eutectic solvent systems were designed and synthesized with lithium bromide and organic alcohols. The DES system suitable for efficient dissolution of wool was found, and the effects of solvent type, reducing agent β-mercaptoethanol (β-ME) dosage (the mass ratio of reducing agent to wool), temperature, solid-liquid ratio (ratio of wool mass (g) to solvent volume (mL)) on the extraction rate of keratin and molecular weight were investigated. The DES system's weak interaction force were analyzed using Quantum chemistry theory simulation and Kamlet-Taft solvatochromic parameters. The dissolution mechanism of lithium bromide in wool was analyzed. The results showed that the LiBr-ethylene glycol (EG) system could maintain the integrity of the internal structure of wool keratin to the greatest extent, break the hydrogen bond network in wool, and realize the weak damage deconstruction of wool. Under the optimal conditions of n (LiBr)∶n (EG) = 1∶4, β-ME dosage 6%, temperature 85 ℃, solid-liquid ratio 1∶20, solution time 0.5 h, the extraction rate of wool regenerated keratin was 58.58%, and the molecular weight was concentrated in 4.50×10⁴—6.62×10⁴.