In this study, a composite adsorbent, layered double hydroxide (LDH)-coated attapulgite (LDH-AP), was synthesized and characterized. Its potential application for LDH stabilizer and phosphate (P) removal from aqueous solution was evaluated using the batch mode and continuous mode in a packed bed column. The batch experiments revealed that the data of P adsorption onto LDH-AP could be well described by the Freundlich equation, and the maximum adsorption capacity was estimated to be 6.9 mg/g. The column experiments were conducted in the tap water and the results indicated that the competing anions could slightly decrease phosphate removal. The saturated column was regenerated by 0.2 mol/L of NaOH and the regenerated column was examined for its reuse in phosphate removal. The results of this study suggested that attapulgite could be used as an applicable stabilizer of LDH and LDH-AP could be potentially used as a promising filtration medium for phosphate removal.