Carbonaceous material for the removal of fluoride ions from water was prepared from coffee grounds (CGs) by calcination and subsequent HCl treatment. The characteristics of the CGs, including the surface area, mean pore diameter, pore volume, and surface functional groups were determined, and the morphological characteristics were evaluated using scanning electron microscopy. The adsorption isotherms, saturated amount of fluoride ions adsorbed, and the effect of contact time and temperature on the adsorption of fluoride ions were investigated for a sample of tap water. The specific surface area of CG calcined at 600° (CG600) was larger than that of CGs calcined at 400, 800, and 1000°. Phenolic, lactonic, and carboxyl groups were detected on the CG600 surface. The adsorption capacity of the carbonized CGs for fluoride was ranked in the order CG400 < CG1000 < CG800 < CG600 (where the numeral indicates the carbonization temperature), whereas virgin CG and CG600-NAT (not treated with hydrochloric acid solution) did not exhibit any adsorption ability for fluoride ions. The amount of fluoride ions adsorbed onto CG600 increased with increasing temperature and was consistent with chemical adsorption. The mechanism of adsorption of fluoride ions onto CG600 proceeded via ion exchange with chloride ions (1:1) present on the surface of CG600. The adsorption isotherms were fitted to the Freundlich and Langmuir equations. Moreover, CG600 showed an acceptable adsorption capacity for fluoride ions present in tap water.