The removal and recovery of phosphate from water by calcium-silicate composite (CSC) and alkali-treated calcium-silicate composite (ASC) was investigated. ASC had a higher specific surface area and total pore volume, and exhibited better performance of phosphate adsorption than CSC. In the batch mode adsorption studies, the isotherm adsorption experiments data fitted well the Langmuir isotherm model and the maximum adsorption capacities were 120 and 73.0 mg/g for ASC and for CSC, respectively. For the kinetic study, the experimental data fitted very well the pseudo-second-order kinetic model. The uptake of phosphate could be performed well over a wide pH range, from 3.0 to 13.0 for ASC and from 4.0 to 13.0 for CSC. The adsorption of phosphate by ASC was very selective even with 10 times higher concentration of other coexistent anions. For the adsorption of low phosphate concentration (10 mg/L), ASC could efficiently remove phosphate at the dosage of 0.8 g/L, while CSC was even difficult to remove phosphate at the dosage of 4.0 g/L. Phosphate fractionation results and FTIR spectra showed that phosphate-Ca complex was formed through phosphate adsorption process. The adsorbed phosphate could be successfully desorbed by 2% citric acid solution, indicating that the adsorbent after adsorbed phosphate could be reusable as fertilizer in the agricultural field.