In this study, the adsorption capability of Fe-HT3.0 for nitrite and nitrate ions in a binary solution system was evaluated. It was found that the amount of nitrite and nitrate ions adsorbed in a single solution (1.19 and 1.27 mmol/g, respectively) was higher than that in a binary solution (0.36 and 0.90 mmol/g, respectively). Equilibrium adsorption was attained within 6–24 h. The adsorption data were fitted to a pseudo-second-order model (correlation coefficient: 0.999), and indicated that the adsorption of both nitrite and nitrate ions is controlled by chemical sorption. Additionally, the binding energies before and after the adsorption of nitrite and nitrate ions in the binary solution system were measured. After adsorption, new nitrogen peaks (approx. 399 and 403 eV) were detected. The results of this study show the potential of Fe-HT3.0 for the removal of nitrite and nitrate ions from aqueous solution systems.