Triphosphate (TPP) is an important form of phosphate pollutants while its removal investigation has been just started now. This research examined the removal of triphosphate using Mg 2−x Ca x FeCl-LDH (x=0–2) as absorbents. We found that the removal of triphosphate over Mg 2 FeCl-LDH mainly underwent the surface adsorption and the near-edge intercalation, with the practical removal amount (9–11mg(P)/g) corresponding to 10–15% of the theoretical one. In contrast, Ca 2 FeCl-LDH removed a higher amount of triphosphate (56.4mg(P)/g). The comprehensive analysis of the triphosphate-uptake products with XRD/XPS/FTIR reveals that Ca 2 FeCl-LDH dissolves first and then released Ca 2+ ions react with triphosphate (TPP) to form insoluble Ca-TPP precipitate. Combination of these two different removal mechanisms enables Mg 0.5 Ca 1.5 FeCl-LDH to take up 84.2mg(P)/g from aqueous solution under similar conditions.