Wastewater from industries can contain excessive phosphate anions to cause eutrophication of lakes and rivers. The calcium iron-based layered double hydroxides (CaFe-LDHs) can improve immobilization the migration of phosphate anions in anti-eutrophication. In this study, we developed an efficient structure for the selective uptake of phosphate anions in aqueous solution on CaFe-LDHs. We also discuss removal mechanism of anions by the CaFe-LDHs related with structure modulation variation that happens during calcination process.