Uptake of inorganic Tl(I) and dimethylthallium, (CH3)2Tl+, by Chlorella spp. (Chlorophyta) and the diatom Stephan-odiscus hantzschii (Heterokontophyta) were measured using radio-tracer techniques in water from Lakes Erie and Superior (North America). Uptake of both Tl(I) and dimethylthallium was bioactive. Uptake of [204Tl]-Tl(I) was greater in Lake Superior water than in Lake Erie water due to the greater K content in Lake Erie that inhibits Tl(I) uptake by phytoplankton but not that of [204Tl]-dimethylthallium. Volume-based bioconcentration factors for Tl(I) after 72 h of exposure were 5 × 104 and 1.1 × 104 for Chlorella sp. and S. hantzschii; for dimethylthallium they were 7.8 × 102 and 8.3 × 103. Both Tl(I) and Tl(III) were concentrated similarly by Chlorella spp. These results suggest that chlorophytes, but not diatoms, accumulate Tl(I) to a greater extent than dimethylthallium. Greater bioaccumulation factors of inorganic Tl are possible in waters containing low amounts of K+; water quality guidelines seeking to protect biota from deleterious effects of Tl should consider the role of K.