According to previous research on polyhydroxy-iron-modified coal-bearing kaolin for the removal of anionic dyes, we first performed a ball milling treatment and then modified the kaolin samples with polyhydroxy-iron to prepare a highsurface-area adsorbent. This process not only increased the surface area up to 100 m 2 g À 1 while successfully avoiding hightemperature calcination and acid treatment but also significantly increased the fluoride adsorption performance in terms of the removal rate, which reached 90 %. Compared with the removal rate of raw kaolin (11 %), that of polyhydroxy-iron-modified coal-bearing kaolin (without ball milling) was ∼ 44 %. Various adsorption conditions that affect the adsorption capacity of the adsorbent were investigated, including the adsorption time, initial solution pH and initial fluoride concentration. The effect of the initial pH showed a wide (pH = 6-8) application range. The adsorption kinetics of fluoride fit well with the pseudosecond-order kinetic model, and the equilibrium data can be well described by the Freundlich adsorption model.