The semiconductor, electroplating, metallurgy, and ceramic industries discharge high concentration fluoride containing wastewater, making fluoride pollution in natural water a global problem.Thus, Zn?Mg?Al LDO is a good adsorbent material. Under different reaction temperatures of n(Zn2+)/n(Mg2+)/n(Al3+), Zn?Mg?Al LDH was synthesized by co?precipitation method, and Zn?Mg?Al?LDH was calcined at different temperatures to obtain Zn?Mg?Al?LDO. X?ray diffraction (XRD), scanning electron microscopy (SEM), Fourier transform infrared spectroscopy (FT?IR) and BET specific surface area testing methods were used to study the structure and properties of Zn?Mg?Al LDO. The adsorption experiment was conducted on 50 mL of NaF solution with an mass concentration of 20.0 mg/L to investigate the performance of Zn?Mg?Al LDO in adsorbing and removing fluoride ions. The results showed that the Zn?Mg?Al LDO prepared under the conditions of n(Zn2+)/n(Mg2+)/n(Al3+)=2∶1∶1, reaction temperature of 75 ℃, and calcination temperature of 400 ℃ exhibited the best adsorption and removal performance of fluoride ions, with an adsorption and removal rate of 85.39%. Zn?Mg?Al LDO has characteristic peaks of hydrotalcite, good crystal structure, and a layered structure. Zn?Mg?Al LDO is a mesoporous material with a specific surface area of 103.15 m2/g. In addition, the kinetics and adsorption mechanism of the adsorption process were also studied. The results indicate that the adsorption process follows the Langmuir adsorption isotherm and quasi second?order kinetic equation.