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Soil and water contaminated with arsenic (As) pose a major environmental and human health problem in Bangladesh. Phytoremediation, a plant-based technology, may provide an economically viable solution for remediating the As-polluted sites. The use of indigenous plants with a high tolerance and accumulation capacity for As may be a very convenient approach for phytoremediation. To assess the potential of native plant species for phytoremediation, plant and soil samples were collected from four As-contaminated (groundwater) districts in Bangladesh. The main criteria used for selecting plants for phytoremediation were high bioconcentration factors (BCFs) and translocation factors (TFs) of As. From the results of a screening of 49 plant species belonging to 29 families, only one species of fern (Dryopteris filix-mas), three herbs (Blumea lacera, Mikania cordata, and Ageratum conyzoides), and two shrubs (Clerodendrum trichotomum and Ricinus communis) were found to be suitable for phytoremediation. Arsenic bioconcentration and translocation factors > 1 suggest that these plants are As-tolerant accumulators with potential use in phytoextraction. Three floating plants (Eichhornia crassipes, Spirodela polyrhiza, and Azolla pinnata) and a common wetland weed (Monochoria vaginalis) also showed high BCF and TF values; therefore, these plants may be promising candidates for cleaningup As-contaminated surface water and wetland areas. The BCF of Oryza sativa, obtained from As-contaminated districts was > 1, which highlights possible food-chain transfer issues for As-contaminated areas in Bangladesh.