Sediment samples were collected from the vicinity of the abandoned South Terras uranium mine in south-west UK and analysed for uranium and (226)Ra to explore their geochemical dispersion. The radioactivity concentrations in the sediment samples were measured using alpha spectrometry for uranium, and gamma spectrometry for radium. Sequential chemical extraction was applied to selected sediments in order to investigate the speciation of the radionuclides and their association with stable elements. The activity ratio of the uranium isotopes was used to explore the mobility of uranium, and scanning electron microscopy (SEM) and electron microprobe analysis (EMPA) were used to characterise the sediments. The radiochemical results identified two locations with enhanced radioactivity, so two samples from these locations were further investigated. The geochemical distribution of the radionuclides in these two samples varies within the five operationally-defined fractions. In one sample, the majority of the uranium was released from the 'carbonate' fraction, followed by the organic fractions. Similarly, in the second sample, the uranium was mainly resealed from the carbonate fraction, although a considerable percentage associated with the resistant fraction. The fractionation trend of radium noticed to show some similarities to that of barium, as expected from the similarity in their chemistries. Geochemical distributions of the stable elements, such as Mn, Ti and As, were different in the enhanced radioactivity samples. The activity ratio of (234)U/(238)U shows different trends in the two sediments, signifying the impact of organic matter and/or the exchange between water and sediment. SEM and EMPA analysis identified uranium-bearing phases in association with potassium, calcium, iron, manganese and arsenic.