The experimental results for the analysis of aluminum hydrolysis species with PACls (polyaluminum chloride) prepared by different basicity (r value) showed that monomeric Al species were reduced while polymeric Al species were increased with an increase in basicity for PACls. The PACl with 2.2 of r value contained the highest amount of polymeric Al species. According to the experimental results for the phosphorus removal, the alum and PACl (r=0), which consisted of mainly monomeric Al species, were the most effective for phosphorus removal. Therefore, it was concluded that the Al coagulant containing higher amount of monomeric or lower molecular Al species would be more beneficial for phosphorus removal.