In this paper, we report a simple chemical method for the preparation of CaO loaded mesoporous Al₂O₃ based adsorbents, which can be used for fluoride removal from water. The synthesized adsorbents were characterized by using powder X-ray diffractometer, N₂ adsorption–desorption surface area and pore size analyzer and high resolution transmission electron microscope. CaO loaded mesoporous aluminas exhibited poor crystalline mesoporous structure having γ-Al₂O₃ phase. The fluoride removal capacities of the synthesized adsorbents were evaluated using batch adsorption studies. Kinetic data revealed that, the fluoride sorption on 20 wt.% CaO loaded mesoporous Al₂O₃ was rapid, and ~90% fluoride removal was achieved within 15 min. CaO loaded mesoporous Al₂O₃ showed higher fluoride adsorption capacity (137 mg/g) and faster kinetics than mesoporous Al₂O₃.