In this effort, hydroxyapatite (HAp)-implanted cerium-based metal organic frameworks (Ce-BTC MOFs) incorporating alginate (Alg) and chitosan (CS) as HAp-Ce-BTC MOFs@Alg-CS beads (biohybrid beads) were developed for effective fluoride remediation. The defluoridation capacity (DC) of biohybrid beads was investigated in relative to the initial ion concentration, shaking time, biohybrid beads dosage, co-ions, temperature, and solution pH. Adsorption kinetics, thermodynamic and isotherm models were exploited to compare the experimental data. The developed biohybrid beads showed a high DC of 4865 mg F − kg −1 under the conditions of 20 min of contact time at 25 °C with a 0.1 g dosage. The instrumentation results such as FTIR, SEM, EDAX, elemental mapping, TGA, DTA, and XRD analysis evidenced that biohybrid beads adsorb fluoride through electrostatic attraction and complexation mechanism. Overall, the biohybrid beads for fluoride adsorption is a spontaneous process with an endothermic nature. Adsorption kinetics and isotherms experimentation results were soundly fit with the pseudo-second-order kinetics and Langmuir models, respectively. The field and recyclability studies of biohybrid beads results exhibit their application under field atmosphere and regeneration ability.