In the present study, the phosphate adsorption abilities of granular materials, gibbsite (GB) and cerium hydroxide (CE), granulated with ethyl cellulose and ethanol, were investigated. For suitable granular conditions using GB or CE, the percentage of binder and amount of solvent were 10% and 3.25 mL/5 g for GB and 7.5% and 2.50 mL/5 g for CE. The amount of phosphate adsorbed by granular GB or CE was similar to that adsorbed by powdered GB or CE. The adsorption isotherms of phosphate were also similar for the granular and powdered materials. The results of a column experiment showed that when GB was used, the suitable concentration of sodium hydroxide as the desorption solution was 2 mmol/L. In these experiments, the amount of phosphate adsorbed was 31.4 mg/g, the amount of phosphate desorbed was 25.3 mg/g, and the recovery percentage was 80.5%. In contrast, when CE was used, the suitable concentration of sodium hydroxide was 500 mmol/L; the amount of phosphate adsorbed was 77.7 mg/g, the amount of phosphate desorbed was 57.8 mg/g, and the recovery percentage was 74.4%. Results also indicate that granular GB and CE could be used at least five times in a column without loss of absorption or desorption abilities. Moreover, granulation of GB and CE is possible using ethyl cellulose and ethanol.