Hyperbilirubinemia could be treated effectively by hemoperfusion. Electrospinning fiber mat had been reported to be applied in the hemoperfusion field owing to its higher surface area. BSA, as one of the natural carrier proteins for bilirubin, can not only selectively adsorb bilirubin but also improve the hemo-compatibility of biomaterials. In this work, functionalized polyethersulfone (PES) electrospun fiber mat was prepared by immobilizing BSA on the surface to remove bilirubin efficiently, in which polydopamine (PDA) acted as an active coating for further modification. The physicochemical characteristics of the PES fiber mat surface were analyzed in detail, indicating that the PDA layer was coated successfully; furthermore, BSA immobilization was also studied. The adsorption experiments demonstrated that PES/PDA-BSA had an excellent adsorption capacity (192.38 mg/g), a short adsorption equilibrium time (1.5 h), and a good selectivity. The adsorption mechanism was analyzed by adsorption kinetics and isotherm models. In addition, dynamic adsorption revealed that PES/PDA-BSA had a shorter equilibrium time for bilirubin, i.e., about 30 min. The selective adsorption of PES/PDA-BSA demonstrated a preferable selectivity toward bilirubin, whether in a single or a multicomponent system, even in a serum system. Further, hemolysis and coagulation assays, as well as protein adsorption, exhibited good blood compatibility. Therefore, this study provided a promising strategy to fabricate a selective adsorbent for bilirubin. (C) 2018 Elsevier B.V. All rights reserved.