The superior removal selectivity of hydrated zirconium oxide nanoparticle-impregnated porous anion exchange resin (ZAE) highlights its use as phosphate removal adsorbent. However, most research examines selective phosphate removal performance using randomly determined single content of hydrated zirconium oxide, and thus the use of the ZAE in real applications remains limited. Therefore, this study aimed to investigate the selective phosphate removal performance of ZAE with different content of hydrated zirconium oxide nanoparticle (HZO NP, represented by zirconium content) by considering various conditions. A molybdate intermediate method was devised to fabricate ZAE with high loaded HZO by weakening the Donnan exclusion to HZO precursors produced from the fixed positively charged host. Consequently, the resultant ZAE was characterized by 17.8 wt% of zirconium. ZAE exhibited an increased selectivity to phosphate against competing ions in the synthetic and simulated real water matrices for both batch and fixed-bed modes as the zirconium content of ZAE increased. High performance was retained, and regeneration led to possible reusability. The linear correlation between selective phosphate removal performances and zirconium content indicates that the zirconium content is a fundamental factor determining the ZAE phosphate adsorption removal. The HZO NPs within ZAE slow adsorption kinetics by blocking AE pores and provide specific adsorption sites for phosphate removal by inner-sphere complexation.