Polymeric-coated ferromagnetic particles with an absorbed layer of octyl(phenyl)-N,N-diisobutylcarbamoylmethylphosphine oxide diluted by tributyl phosphate are being evaluated for application in the separation and the recovery of low concentrations of americium and plutonium from nuclear waste solutions. Due to their chemical nature, these extractants selectively complex americium and plutonium contaminants onto the particles, which can be recovered from the waste solution using a magnet. The effectiveness of the extractant-absorbed particles at removing transuranics (TRU) from simulated solutions and various nitric acid solutions was measured by gamma and liquid scintillation counting of plutonium and americium. The HNO3 concentration range was 0.01 to 6 M. The partition coefficients (Ka) for various actinides at 2 M HNO3 were determined to be between 3000 and 30,000. These values are larger than those projected for TRU recovery by traditional liquid/liquid extraction. Results from transmission electron microscopy indicated a large dependence of K-d On relative magnetite location within the polymer and the polymer surface area. Energy disperse spectroscopy demonstrated homogeneous metal complexation on the polymer surface with no metal clustering. The radiolytic stability of the particles was determined by using Co-60 gamma irradiation under various conditions. The results showed that K-d more strongly depends on the nitric acid dissolution rate of the magnetite than the gamma irradiation dose. Results of actinide separation from simulated high-level. waste representatives of that at various DOE sites are also discussed.