Iron-based layered double hydroxides (M2+(a)Fe3+(b) (OH)2(a+b) CO3(2-) b/2mH2O) were synthesized. Removal of phosphate by the compounds was studied from the viewpoint of buffering pH effect of the compounds and buffering capacity of solution. The compounds released metal cations (Mg2+, Ca2 , Fe3+) and/or their hydroxides responding to various water environments due to their buffering pH function. The released cations and/or hydroxides worked effectively as coagulants for the phosphate removal. The removal of phosphate depended on the buffering capacity of the solution that is the function of the solution pH and the concentration of phosphate. The removal of phosphate from the solution with small buffering capacity followed a Langmuir-type isotherm. The removal of phosphate from the solution with larger buffering capacity was largely increased. The removal of phosphate by the compounds was analyzed based on the model describing the buffering pH effect of the compounds from which the amount of released cations (CB) can be determined. The removal was well correlated with the amount of dissolution of the compounds, CB. The mechanism of phosphate removal was examined based on the removal efficiency (mol of removed phosphate/mol of released alkali). The efficiencies showed below one in the solution with large buffering capacity and above one in the solution with small buffering capacity. The efficiency below one showed the removal of phosphate through coagulation by the released metal cations and hydroxides. The successful removal of dilute phosphate (0.2mg P/l) from the drain water was also demonstrated.