The ability of the alum-impregnated activated alumina (AIAA) for removal of fluoride from water through adsorption has been investigated in the present study. All the experiments are carried out by batch mode. The effect of various parameters viz. contact time, pH effect (pH 2–8), adsorbent dose (0.5–16 g/l), initial fluoride concentration (1–35 mg/l) has been investigated to determine the adsorption capacity of AIAA. The adsorbent dose and isotherm data are correlated to the Bradley equation. The efficacy of AIAA to remove fluoride from water is found to be 99% at pH 6.5, contact time for 3 h, dose of 8 g/l, when 20 mg/l of fluoride is present in 50 ml of water. Energy-dispersive analysis of X-ray shows that the uptake of fluoride at the AIAA/water interface is due to only surface precipitation. The desorption study reveals that this adsorbent can be regenerated following a simple base–acid rinsing procedure, however, again impregnation of the regenerated adsorbent (rinsed residue) is needed for further defluoridation process.