A series of Mg/Al/Zr ternary hydrotalcite-like materials with different Zr4+ contents were prepared by co-precipitation method. The phosphate adsorption performances of these materials were also studied. The structural and textural properties of these materials were characterized by XRD, DRIFTS and nitrogen adsorption-desorption experiments. The effects of initial pH and competitive anions on the phosphate adsorption capacity were also investigated. The results show that the addition of Zr4+ enhanced the positive charge density of the hydrotalcite-like layer and increased the interlayer spacing, which was beneficial to the adsorption of phosphate anions. The phosphorus adsorption process of Mg/Al/Zr hydrotalcite-like followed the pseudo-second-order kinetic model. The adsorption isotherm followed the Langmuir model. As the molar ratio of (Zr4+)/(Al3++Zr4+) was 0.3, the theoretical saturated adsorption uptake of Mg/Al/Zr hydrotalcite-like reached the maximum value of 76.6 mg/g that was 28.7% higher than that of Mg/Al hydrotalcite. The acidic environment was conducive to the adsorption of phosphate, while the competitive adsorption of divalent anions significantly reduced the phosphorus adsorption performance. The phosphorus adsorption of Mg/Al/Zr hydrotalcite-like was the result of the synergistic effect of electrostatic attraction and anion exchange.