Freezing-induced chemical crosslinking to fabricate nanocellulose-based cryogels for efficient bilirubin removal

•A novel approach is developed to fabricate robust MFC cryogels by using freezing-induced chemical crosslinking.•The chemical cross-linking mechanism behind the freezing process has been investigated in detail.•The obtained MFC cryogels present excellent mechanical performance and outstanding chemical stability under harsh conditions.•The PEI-MFC cryogel reveals a record-high bilirubin adsorption capacity of 351.49 mg/g at the present of 40.0 g/L BSA.•The cryogel-packed column can remove bilirubin continuously under simulated perfusion conditions.