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• Magnetic biosorbents (PMCCs) were designed and fabricated by radical polymerization. • PMCCs had specific morphological and molecular structure for ciprofloxacin removal. • PMCCs exhibited excellent adsorption capacity of 527.93 mg·g−1 for ciprofloxacin. • The adsorption mechanisms of ciprofloxacin by PMCCs were systematically elucidated. • PMCCs displayed rapid separation and favorable reusability. Magnetic biosorbents with specific morphological and molecular structure (PMCCs) were designed for the removal of ciprofloxacin (CIP) from water. Radical polymerization method was applied to immobilize the designed polymer brushes onto core-shell shaped magnetic microspheres to fabricate PMCCs. PMCCs exhibited a maximum adsorption capacity of 527.93 mg·g−1, which is much higher than reported adsorbents, owing to the complete stretch of polymer brushes and increased active sites as well as enhanced interaction. The investigation on the adsorption behavior of PMCCs for CIP manifested that CIP adsorption well fitted the Langmuir isotherm model and pseudo-second-order kinetic model. The calculated thermodynamic parameters suggested that CIP adsorption onto PMCCs was spontaneous and exothermic. Further recycling experiments showed a loss of less than 20% in the CIP adsorption capacity after five times, demonstrating the reusability of the as-designed biosorbents. [ABSTRACT FROM AUTHOR]