In this current study, aminated graphene oxide (AGO) doped on alginate (Alg) matrix offers AGO@Alg hybrid spheres was developed to investigate its potential for retention of fluoride from water. The sophisticated characterization methods likely TGA, SEM, XPS and FTIR studies of AGO@Alg hybrid spheres were attained to recognize its physicochemical properties like thermal stability, morphology, elemental binding energy and functional groups determination. The responsible parameters for fluoride adsorption on AGO@Alg hybrid spheres were optimized under a batch mode to achieve improve defluoridation capacity (DC). The developed AGO@Alg hybrid spheres follow the electrostatic interaction mechanism on fluoride removal. The adsorption isotherms (Langmuir, Temkin, Dubinin–Radushkevich (D–R) and Fruendlich models), kinetics (reaction and diffusion based models) and thermodynamic parameters (ΔS°, ΔG° and ΔH°) were investigated at 303, 313 and 323 K. To minimize the cost-effectiveness of AGO@Alg hybrid spheres the reusability test was carried out. The suitability of AGO@Alg hybrid spheres was also analyzed for the fluoride contaminated field sample taken from fluoride prevalent village.