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 exhib-ited poor crystalline mesoporous structure having c-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.