Pure HEU-type zeolite (heulandite) crystals were allowed to interact with Sr2+ cations in aqueous solution. The powdered solid experimental products obtained from batch-type sorption experiments, using solutions of Sr2+-concentrations between 10 and 1000 mg/l, were investigated using INAA, RI-XRF and SEM-EDS. The Sr uptake by the mineral which can adequately be described with a Freundlich-type isotherm, varies from 3.14 to 6.22 mg/g. The distribution coefficients increase progressively by decreasing the solutions concentration reaching a value of 1800 ml/g. The investigated zeolite interacts with Sr2+ cations through ion exchange reactions and initial exchangeable Ca2+ cations are replaced into the structural micropores. However, in the best case, only ca. 43% of the theoretical CEC can be covered because of the limited availability of the extra framework Ca2+ cations that can be removed from the lattice under ambient treatment conditions. The XPS investigation of Sr-loaded single crystals indicated that adsorption of Sr2+ cations on the outer surface also occurs while surface precipitation phenomena must be excluded. Similar surface analyses by means of12C-RBS showed that the Sr depth-distribution at near-surface layers is quite homogenous in contrast to a previous relevant study revealing an intense surface Sr-accumulation on a natural Ca-zeolite of different structural characteristics (scolecite).