Xonotlite was synthesized and tested for phosphate removal and recovery from synthetic solution in a batch mode. The effects of pH, initial calcium concentration, bicarbonate concentration on phosphate removal through crystallization were examined. The morphology and X-ray diffraction (XRD) patt of xonotlite before and after crystallization confirmed the formation of crystalline hydroxyapatite. The results indicated that, the crystallization product had a very high P content (＞ 10%), which is comparable to phosphate rock at the dosage of 50-200 mg xonotlite per liter, with a maximum P content of 16.7%. The kinetics of phosphate removal followed the second-order reaction equation. The phosphate removal ability increased with increasing pH. The precipitation of calcium phosphate took place when pH is higher than 7.2, whereas the crystallization occurred at pH 6.0. A high calcium concentration can promote the removal of phosphate via crystallization, while a high bicarbonate concentration also enhanced phosphate removal through that it increased the pH and thus induced the precipitation process. When xonotlite was used to remove phosphate from wastewater, the removal efficiency could reach 91.3% after 24 h reaction time, with removal capacity 137 mg/g. The results indicated that xonotlite might be used as an effective crystal seed for the removal and recovery of phosphate from aqueous solution.