Environmentally compatible polymeric membrane marine sensors with excellent antiadhesive and antibacterial properties have recently been developed. However, the regeneration abilities of these sensors after fouling have rarely been investigated. Herein, a novel strategy for preparation of a regenerable antibiofouling coating via surface modification of a dual-functionalized magnetic composite is proposed. A zwitterionic polymer (i.e., poly(sulfobetaine methacrylate)) and a quaternary ammonium compound (i.e., 3-trimethoxysilylpropyl octadecyldimethyl ammonium chloride) are coated on the surface of Fe3O4 microspheres for antiadhesion and bacterial inactivation, respectively. The antifouling magnetic composite can readily be modified on the sensor's surface via the magnetically assisted self-assembly technology. Using a polymeric membrane calcium ion-selective electrode as a model sensor, the protection layer-coated electrode shows the markedly improved antibiofouling activities as compared to the unmodified sensor. More importantly, by altering the direction of the external magnetic field, the antifouling coating can easily be removed after fouling along with the removal of the adsorbed bacterial cells from the electrode's surface, which is followed by re-modifying a fresh coating for regeneration of the antifouling electrode. The proposed methodology for fabrication of a regenerable antibiofouling coating is promising to improve the durability of a marine sensor.