Zn-Fe layered double hydroxide with chloride intercalation (ZFCL) was synthesized by a coprecipitation method at room temperature. ZFCL was characterized by N 2 adsorptiondesorption isotherms, X-ray diffraction, scanning electron microscope, Zeta-sizer analyzer, X-ray photoelectron spectroscopy, and Fourier transform infrared spectroscopy. The results showed that ZFCL had large surface area and layered structure. The maximum adsorption capacity of ZFCL was 150.6 mg/g at 25°C. That was higher than most other adsorbent which were reported. The kinetic data were described better by the pseudo-second-order adsorption kinetic rate model. The adsorption isotherm on the adsorbent was described by Langmuir, Freundlich, and Sips models at pH 6 and followed the fitting order: Sips >Freundlich>Langmuir. Thermodynamic analyses indicated that the phosphate adsorption on ZFCL was endothermic and spontaneous in nature. The sequence of coexisting cations and anions competing with phosphate was Ca 2+ > Mg 2+ > Na + and SO 4 2− > NO 3 − > Cl − . ZFCL can be regenerated by the sequential use of NaOH and ZnCl 2 . The adsorption capacity remained high as 108.6 mg/g after regeneration of 3 times. The results of zeta potential, Fourier transform infrared spectroscopy, and X-ray photoelectron spectroscopy analyses indicated that the phosphate adsorption mechanisms involved ion exchange, Zn 3 (PO 4 ) 2 precipitation, and the formation of inner-sphere complex via replacement of surface hydroxyl groups by phosphate.