The adsorption of fluoride by chitosan magnetic microspheres of loading lanthanum metal (CTS-La) was investigated in this study. The chitosan magnetic materials were prepared by organically-linking technique. The effects of pH, the reaction time, the initial concentration, dosage and temperature on the removal rate were studied to determine to the optimum operating parameters. The experimental results show that CTS-La is a black particle shape material with magnetism. The magnetic microspheres have high adsorption ability for fluoride, and the maximum removal of F- was 98.4% under the operating parameters of the initial fluoride concentration 10mg/L, pH=2-3,the reaction time 60minutes, dosage 0.1g, temperature 318K. . The equilibrium sorption data are fitted reasonably well in Langmuir and Freundlich isotherm model, and the correlation coefficients (R2) were Langmuir’s correlation and 0.9997 respectively.