Two adsorbents, magnesium aluminum calcined hydrotalcite (MgAl LDO) and magnesium aluminum iron calcined hydrotalcite (MgAlFe LDO), were synthesized by coprecipitation method, and characterized by X?ray powder diffraction (XRD) analysis, scanning electron microscopy (SEM) analysis, Fourier transform infrared spectroscopy (FT?IR) analysis and BET specific surface area test analysis, etc. The adsorption performance of the two adsorbents for fluoride in wastewater was also studied. The effects of the ratio of metal substances, calcination temperature, initial mass concentration of F^-, and adsorbent dosage on the removal efficiency of fluoride in wastewater were investigated. The results showed that MgAlFe LDO had a uniform pore structure distribution, a large specific surface area, and a higher adsorption capacity for fluoride in wastewater than that of MgAl LDO. When n (Mg²⁺)/n (Al³⁺)/n (Fe³⁺)=3.0∶0.6∶0.4, the initial mass concentration of F^- was 20 mg/L, the calcination temperature was 300 ℃, and the dosage of MgAlFe LDO was 0.4 g, the removal effect of fluoride in wastewater was optimal. After 2 hours of reaction, the removal rate of fluoride in the wastewater was 98.35%.