Removal of low-concentration fluoride in natural water is an important issue all over the world. Japan is a volcanic country with many hot springs, and the removal of low-concentration fluoride from hot spring drainage is desired. In this study, we attempted to prepare a novel adsorbent with high selective removal ability of fluoride from zircon sand using mechanochemical treatment, and applied it for removing fluoride from hot spring water. Mechanochemical treatment of zircon sand was carried out using a planetary ball mill, and fluoride removal of the product was examined using fluoride aqueous solution and hot spring water. The hot spring water is collected from one of the hot spring in Japan, and a typical sulfuric acid hot spring water pH 2 including high contents of SO4 2-(12000 mg  L -1 ) and Cl -(5000 mg  L -1 ) with 11 -15 mg  L -1 of fluoride ion. Regardless of ball sizes, with increasing the mechanochemical treatment time to 10 min, the removal ability of the product for fluoride increases, and then be almost constant. With decreasing pH of the solution to 2, the adsorption amount increases, and then be almost constant. With increasing the temperature of the solution, the adsorption amount decreases, while the rate of adsorption increases and the amount increases. The adsorption isotherm at pH 2 follows much better Langmuir model than Freundlich model, and the calculated maximum adsorption amount is 0.11 mmol  g -1 . Fluoride can be adsorbed selectively from hot spring water below Japanese effluent standard for fluoride (8.0 mg  L -1 ).