A new magnetic adsorbent material, called magnetic polyamine-epichlorohydrin (MPE) resin, was prepared by attaching activated magnetite to the outer surface of polyamine-epichlorohydrin resin beads. Experiments were carried out in the presence of a 0.3-tesla magnetic field to investigate the removal of actinides (plutonium and americium) from pH 12 wastewater using this new resin. The results demonstrated that the MPE resin has a significantly enhanced capacity for actinides over conventional ferrite-based surface complexation adsorption processes (where no field is applied) and over traditional high-gradient magnetic separation (HGMS) processes that remove suspended particles. This enhancement was attributed to the presence and subsequent removal of suspended actinide nanoparticles through an HGMS effect, with the magnetite acting as a very effective HGMS element. A theoretical analysis verified this supposition by showing that under adequate pHs and particle-particle separations, the attractive long-ranged magnetic force exerted by magnetite on suspended particles of plutonium hydroxide was greater in magnitude than other forces (e.g., van der Waals, electrostatic, viscous, and Brownian forces).