Indian mustard [Brassica juncea (L.) Czern.] transgenics overexpressing ATP sulfurylase (APS plants) were shown previously to have higher levels of total thiols, S, and Se. The present study explores the effect of ATP sulfurylase overexpression on tolerance and accumulation of other metals, both oxyanions and cations, reasoning that some anions may react directly with ATP sulfurylase, while other ions may be bound by its thiol end products. The APS transgenics were compared with wild-type plants with respect to tolerance and accumulation of As, Cd, Cr, Cu, Hg, Mn, Mo, Ni, Pb, V, W, and Zn, supplied individually in agar medium (seedlings) or in hydroponics (mature plants). At the seedling stage, APS transgenics were more tolerant than wild type to As(III), As(V), Cd, Cu, Hg, and Zn, but less tolerant to Mo and V. The APS seedlings had up to 2.5-fold higher shoot concentrations of As(III), As(V), Hg, Mo, Pb, and V, and somewhat lower Cr levels. Mature APS plants contained up to 2.5-fold higher shoot concentrations of Cd, Cr, Cu, Mo, V, and W than wild type. They also contained 1.5- to 2-fold higher levels of the essential elements Fe, Mo, and S in most of the treatments. Mature APS plants showed no differences in metal tolerance compared with the wild type. Overexpression of ATP sulfurylase may be a promising approach to create plants with enhanced phytoextraction capacity for mixtures of metals.