In this study, the development and characterization of a novel adsorbent, iron(III)-coordinated amine-modified poly(glycidylmethacrylate)-grafted densified cellulose (AM-Fe-PGDC), for the removal and recovery of fluoride ions from aqueous solutions is reported. The adsorbent was characterized by FTIR, X-ray diffraction, SEM, TG/DTG, surface area analyzer, and potentiometric titration. The effect of process parameters such as agitation time, concentration, pH, ionic strength, adsorbent dose, and temperature on the extent of fluoride adsorption was investigated. The adsorbent exhibits very high adsorption potential (>99.9%) at an optimum equilibrium pH 7.0. The nonlinear form of a pseudo second-order kinetic model and Langmuir isotherm model adequately described the experimental kinetic and equilibrium data. The thermodynamic parameters showed that the adsorption of fluoride onto AM-Fe-PGDC was feasible, spontaneous, and exothermic. Adsorption experiments were also conducted using a commercial anion exchanger, Duolite-A7, for comparison. Utility of the adsorbent was tested with a simulated industry wastewater sample. Adsorbed fluoride ions were desorbed effectively by 0.1 M HCl.