Analytical techniques were combined with geochemical modelling to study the release mechanisms of pollutants from an abandoned gold mining tailings storage facility near Johannesburg. Inverse modelling of sampled tailings pond water and experimental single extractions using various solutions indicated which combination of naturally occurring leaching solutions were likely to give rise to the observed pond water quality. The potential fate of metals in the pond was predicted by modelling the formation of efflorescent crusts and adsorption onto hydrated iron oxide minerals.