a b s t r a c tThis study investigates the effects of aluminum (Al) and F interactions on the coagulation behaviors of Al salts, i.e., AlCl 3 and polymer aluminum chloride (PACl) at different basicity (B) towards fluoride. These coagulants achieve the optimum fluoride removal over pH 6-7, and PACl exhibits higher removal efficiency than AlCl 3 does over pH 4-9. The removal of fluoride is positively correlated with the content of either Al 13 or Al b in Al-based coagulants over pH 4-9 and increases in the order: PACl 2 > PACl 1 > AlCl 3 . As for PACl, the increased B from 0 to 2.4 improves fluoride removal owing to the elevated ratios of Al b . However, at further increased B to 2.8, the formation of colloidal Al species