Different molar ratios of a Ni/Co binary hydroxide (NiCo82, NiCo91, and Ni100) were prepared and calcined at 270 °C (NiCo82-270, NiCo91-270, and Ni100-270). The properties of the adsorbents and the amount of adsorbed phosphate ions were evaluated. The adsorbents calcined at 270 °C had a nickel oxide structure. The amount of adsorbed phosphate ions, the amount of hydroxyl groups, and the specific surface area of the calcined adsorbents at 270 °C were greater than those of the uncalcined adsorbents. The amount of adsorbed phosphate ions was related to the amount of hydroxyl groups and the specific surface area; the correlation coefficients were 0.966 and 0.953, respectively. The adsorption isotherm data for NiCo91 and NiCo91-270 were fit to both the Freundlich and Langmuir equations. The amount of adsorbed phosphate ions increased with increasing temperature. The experimental data fit the pseudo-second-order model better than the pseudo-first-order model. A neutral pH was optimal for phosphate ion adsorption. In addition, the phosphate ions that were adsorbed onto NiCo91-270 could be recovered using sodium hydroxide, and the adsorbent was useful for the repetitive adsorption/desorption of phosphate ions. Collectively, these results suggest that NiCo91-270 is prospectively useful for the adsorption of phosphate ions from aqueous solutions.