The behaviours of Pu, Am and colloids in feed solutions to the Site Ion-exchange Effluent Plant (SIXEP) at the Sellafield nuclear reprocessing site in the U.K. have been studied. For both Pu and Am, fractions were found to be associated with material in the colloidal size range, with ∼50% of the Pu in the range 1-200 nm. The concentration of soluble Pu (<1 nm) was ∼1 nM, which is very similar to the solubility limit for Pu(V). The soluble Am concentration was of the order of 10-11 M, which was below the solubility limit of americium hydroxide. The size, morphology and elemental composition of the particulates and colloids in the feed solutions were investigated. Magnesium is homogeneously distributed throughout the particles, whereas U, Si, Fe, and Ca were present in localised areas only. Amongst some heterogeneous material, particles were identified that were consistent with hydrotalcite. The distribution of 241Am(III) on brucite (magnesium hydroxide) colloids of different sizes was studied under alkaline conditions representative of nuclear fuel storage pond and effluent feed solution conditions. The morphology of the brucite particles in the bulk material observed by ESEM was predominantly hexagonal, while that of the carbonated brucite consisted of hexagonal species mixed with platelets. The association of 241Am(III) with the brucite colloids was studied by ultrafiltration coupled with gamma ray-spectrometry. For carbonate concentrations up to 10-3 M, the 241Am(III) was mainly associated with larger colloids (>300 kDa), and there was a shift from the smaller size fractions to the larger over a period of 6 months. At higher carbonate concentrations (10-2 M), the Am was predominantly detected in the true solution fraction (<3 kDa) and in smaller size colloidal fractions, in the range 3-100 kDa.