Selenium (Se) plays a role in human health: It is an essential trace element but can be toxic if too much is consumed. The aim of this study was to determine which species of Se are most rapidly taken up and translocated to above-ground plant tissues. Specifically, we wished to determine if organic forms of Se in an exposure solution can contribute to the amount of Se found in shoot tissue. Durum wheat (Triticum turgidum) and spring canola (Brassica napus) were grown hydroponically, and young seedlings were exposed to 0.5 or 5.0 μM Se as selenate, selenite, seleno-methionione, or seleno-cystine for ≤300 min. Canola accumulated more Se than wheat, although the difference depended on Se speciation of the exposure solution. Organic forms of Se were taken up at a greater rate than inorganic forms. When exposed to 5.0 μM Se, the rate of uptake of selenite was 1.5- (canola) or 5-fold (wheat) greater than the rate of uptake of selenate, whereas seleno-methionine was taken up 40- (canola) or 100-fold (wheat) faster and seleno-cystine 2- (wheat) to 20-fold (canola) faster. Plants exposed to seleno-methionine had the highest shoot concentrations of Se even though selenate was more mobile once taken up; in plants exposed to selenate >50% of accumulated Se was translocated to shoot tissue. Because organic forms of Se (especially seleno-methionine) can be readily taken up and translocated to above-ground tissues of wheat and canola, these Se species should be considered when attempting to predict Se accumulation in above-ground plant tissues.