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The interaction between chitooligosaccharides (COS2-6) and bovine serum albumin (BSA) is worthy of investigation, which provides support for improving the physical properties (gelling, foaming, and emulsifying) of food proteins via COS addition and in vivo research on COS bioactivity. Component analysis indicated that COS2 and COS3 were enriched in the COS2-6-BSA precipitate. The fluorescence binding constant (1.73 × 103 M-1), ΔG of isothermal titration calorimetry (-6.7 kJ/mol), and the predicted ΔG of molecular docking (-10 to -5 kJ/m