Electrokinetic soil processing is an emerging technology for decontamination of certain radionuclides, heavy metals, or organic species from soils or slurries. Tests reveal that the process efficiencies in partially saturated kaolinite samples (without contaminants) are high, since water supplied at the anode eventually flushed across the specimens and saturated the deposits. Consolidation settlements are expected in the vicinity of anodes in fine-grained soils, even when both electrodes allow ingress of the water. Uranyl ion at 1000 pCi/g could be effectively removed from kaolinite but the removal efficiency decreased close to the cathode due to the high pH in this region. A yellow uranium hydroxide precipitate was collected at the cathode. Thorium ion, even at 300 pCi/g, could not be efficiently removed throughout the cell because of its high adsorptive capacity, facile hydrolysis, and the precipitation of insoluble hydroxide. Methods are required to prevent hydroxide ion formation by the cathode reduction of water and thus enable extraction of these metal species in soluble forms.