Calculations of radiological risk are required to assess the safety of any potential future UK deep underground repository for intermediate-level and certain low-level solid radioactive wastes. In support of such calculations, contaminant movement and dilution in the terrestrial biosphere is investigated using the physically based modelling system SHETRAN. Two case studies are presented involving modelling of contaminants representing long-lived poorly sorbed radionuclides in the near-surface aquifers and surface waters of hypothetical catchments. The contaminants arise from diffuse sources at the base of the modelled aquifers. The catchments are characterised in terms of detailed spatial data for topography, the river network, soils and vegetation. Simulations are run for temperate and boreal climates representing possible future conditions at a repository site. Results are presented in terms of the concentration of contaminants in the aquifer, in soils and in surface waters; these are used to support the simpler models used in risk calculations.