We investigated effects of the application of a sulfur-modified organoclay (SMOC) at doses of 1%, 3% and 5% (w/w) on the geochemical fractionation of mercury (Hg) and its accumulation by pea and corn in a polluted floodplain soil. Soil Hg was fractionated sequentially to five operationally defined fractions as follows: F1: water soluble Hg; F2: "human stomach acid" soluble Hg; F3: organo-chelated Hg; F4: elemental Hg; and F5: Hg-sulfur-compounds/residual Hg. The high dosage of SMOC caused a decrease of Hg in F3 (18%) and F5 (36-63%), and 6.7 fold increase of Hg in the mobile fraction (MF = F1+F2) as compared to control soil. The transformation of Hg from F5 to the MF in SMOC-treated soil might be due to the associated decrease of soil pH. Pea accumulated more Hg than corn. Mercury contents were larger in roots than in shoots of both plants and increased significantly by a factor of up to 11 by SMOC addition. The potential transformation of Hg from the hardly soluble to the MF by SMOC addition and the associated increase of Hg accumulation by plants imply a great potential of the SMOC for enhancing Hg phytoremediation.