Colloidal particles of CaO were synthesized by the sol-gel method. The particle morphology was characterized by FT-IR, TGA, DTA, and TEM analysis. The ability of the CaO nanoparticles for removal of fluoride from aqueous solution through adsorption has been investigated. All the experiments were carried out by batch mode. The effect of various parameters viz. contact time, pH effect (pH 2-10), adsorbent dose (0.01-0.1 g/100 ml), initial fluoride concentration (10-100mg/1) and competitive ions has been investigated to determine the adsorption capacity of CaO nanoparticles. Almost complete removal (98%) of fluoride was obtained within 30 minutes at an optimum adsorbent dose of 0.6 g/L for initial fluoride concentration of 100 mg/L. The adsorption isotherm was also studied to find the nature of adsorbate-adsorbent interaction.