Surface modification of adsorbents plays a crucial role in its adsorption performance. Furthermore, the most important step in modification is to design the modification groups based on target pollutants. In this study, the phosphate adsorption performance of zirconium hydroxide was enhanced by different ammonium modification as a result of increasing utilization efficiency of adsorption site. The maximum capacity is 155.04 mg/g from the zirconium hydroxide modified by dimethylamine. In comparison with undecorated zirconium hydroxide, the selectivity factors for Cl–, SO42–, and NO3– are all raised by almost 2 times by dimethylamine modification. The mass transfer rate K2 also increase 6 times using N-methylaniline and N-ethylmethylamine. Results from zeta-potential and FT-IR revealed that the enhanced adsorption capacity for phosphate were directly related to the inner-sphere complex and electrostatic interactions (quaternary ammonium groups and phosphate) and ligand exchange (the hydroxyl groups of zirco...