Nano-composites were synthesized by the reaction of waste polystyrene (PS) and KMnO4. The structure of the composite was controlled by the solvent/non-solvent system and the concentration of KMnO4. The FTIR spectra indicated the functionalizadon of PS and the attachment of NMO with the polymer chains. The maximum adsorption capacities (q(max)) were 10,000 and 5000 Bq g(-1), for U and Th respectively. Different but controllable sorption/desorption behaviours were noted between Th and U, which could be promising in the separation of Th and U from their mixture.