A novel starch stabilized Mg/Al LDHs material (S-LDH) was prepared in a facile approach and its fluoride ion removal performance was developed. Characterization of S-LDH was employed by using XRD, FTIR and particle size distribution. The adsorption property was studied through the assessment of adsorption isotherms, kinetic models, thermal dynamics and pH influence. The result shows that a low loading of starch of 10 mg onto LDH could obviously improve fluoride removal rate. The S-LDH had 3 times higher adsorption capacity to fluoride than that of Mg/Al LDH to fluoride. The particle size was smaller and the particle size distribution was narrower for S-LDH than that for Mg/Al LDH. Langmuir adsorption isotherm model and pseudo-second-order kinetic model fitted well with the experimental data. In thermodynamic parameters, the enthalpy (△H0) value was 35.63 kJ mol-1 and the entropy (△S0) value was 0.0806 kJ mol-1K-1. The values of △G0 were negative, implying the adsorption process is spontaneous. S-LDH reveals stable adsorption property in a wide pH range from 3 to 9. The mechanism for fluoride adsorption on S-LDH included surface adsorption and interaction ion exchange.