In this study, amino-functionalized magnetic particles (iron oxide@SiO2-NH2) with core-shell structures were synthesized and evaluated for rapid boron removal from aqueous solutions. The results showed that the specific surface area of the iron oxide@SiO2-NH2 (131.24 m2⋅g−1) increased greatly compared to pure iron oxide (30.98 m2⋅g−1). The adsorption equilibrium was less than 2 h, with an adsorption capacity of 29.76 mg⋅g−1 at pH = 6 at 15 °C. The quasi-second-order kinetic model described the boron adsorption process well, and both the Langmuir and Freundlich models were suitable for characterizing the adsorption isotherms. The zeta potential and XPS analysis before and after adsorption revealed that the main adsorption mechanism was the hydrogen bonding formation between the terminal -NH2 groups of the adsorbent and the boric acid. In addition, the adsorbent still maintained a high adsorption performance after five adsorption–desorption cycles, which illustrated that the iron oxide@SiO2-NH2 may be a potential adsorbent for environmental boron removal treatment.