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Methylmercury (MeHg) and, to a lesser extent, inorganic mercury (IHg) contamination of rice is a global public health concern, but little is known about how soil and grain Hg concentrations respond to elevated CO2 (ECO2), or how ECO2 alters movement of Hg through the soil-plant-grain system. To advance knowledge of how Hg contamination of rice will change in the future, this study explored the effect of elevated CO2 (ECO2, c. 800 ppm) on soil, iron plaque, root, stem/leaf, and grain concentrations of MeHg and IHg. We observed evidence that ECO2 increased accumulation of MeHg, but not IHg, in rice grain. For IHg, ECO2 did not alter its uptake from the soil, translocation through the plant, or concentration in rice grain. However, ECO2 did reduce uptake of IHg from the air into leaf tissues, likely as a result of the reduced stomatal conductivity and thus more limited direct uptake from the air. Methylmercury concentrations in the grain of plants grown at ECO2 were significantly higher than those of plants grown at ambient CO2. Moreover, MeHg concentrations were also elevated in stem/leaf (82 %) and root tissue (37 %) for ECO2 plants, although the root-tissue results were not statistically significant. In contrast, soil MeHg concentrations were virtually indistinguishable between treatments, indicating that higher rice grain MeHg concentrations were not likely due to higher microbial IHg methylation in soil. Plant uptake of MeHg into stem/leaves and grain from the soil was significantly greater in the ECO2 treatment; however, translocation patterns of MeHg within the plant itself did not differ between treatments. Notably, these patterns existed despite consistently lower transpiration in the ECO2 treatment, and thus less mass flow of solute towards and through the plant. Our results indicate that as CO2 concentrations rise, the human health risks related to MeHg in grain will likely increase.