The removal of phosphate from water has attracted increasing attention because of the dominant role of phosphate in eutrophication. In this study, a novel nanoscale hybridized adsorbent, NLC@213, was fabricated by immobilizing nanosized lanthanum carbonate (NLC) into the pores of the macro-porous polyacrylic anion exchanger D213 through an in-situ precipitation method for phosphate adsorption from wastewater. NLC@213 exhibited excellent pH tolerance and possessed a high selectivity for phosphate in the presence of competing anions (Cl − , NO 3 − , SO 4 2− , SiO 3 2− , and HCO 3 2− ) and organic acids (humic, tannic, and gallic acids). The maximum phosphate adsorption capacity reached 53.64 mg P/g at 30 °C. Moreover, fixed-bed column adsorption experiments demonstrated that NLC@213 could effectively treat 2400 bed volumes of real secondary effluent (phosphate concentration decreased from 2.0 to <0.5 mg P/L). The exhausted NLC@213 could be regenerated easily using a binary solution of NaCl (1.5 mol/L)−Na 2 CO 3 (3 mol/L), and no significant capacity loss was observed during the recycling for column adsorption−desorption. The underlying mechanism of phosphate adsorption was investigated by a combination of Fourier-transform infrared, transmission electron microscopy, and X-ray photoelectron spectroscopy, and the formation of LaPO 4 •xH 2 O was suggested to be the main pathway in the separation process of phosphate from real secondary effluent.