Simple SummaryThe goal of this study was to measure the concentrations of four potentially toxic metals in green amaranth (leaves, stems, and roots) collected from 11 sampling sites in Peninsular Malaysia. The danger of the metal concentrations to human health was assessed. The metal levels were highest in the root parts, followed by stems and leafy parts. The positive relationships of metals between plant parts and the habitat topsoils suggested that the green amaranth could be used as a useful biomonitoring agent of Cd, Fe, and Ni pollution. In addition, the green amaranth was also a very promising phytoextraction agent of Ni and Zn and a very promising phytostabiliser of Cd and Fe. This indicates that green amaranth can be used in the phytoremediation of the polluted soils by Cd, Fe, Ni, and Zn. The human health risk assessment for the potentially toxic metals (PTMs) in the leaves of green amaranth indicated that the four metals posed no non-carcinogenic dangers to consumers. However, it is of utmost importance to monitor PTMs in Amaranthus fields periodically.Human health risk and phytoremediation of potentially toxic metals (PTMs) in the edible vegetables have been widely discussed recently. This study aimed to determine the concentrations of four PTMs, namely Cd, Fe, Ni, and Zn) in Amaranthus viridis (leaves, stems, and roots) collected from 11 sampling sites in Peninsular Malaysia and to assess their human health risk (HHR). In general, the metal levels followed the order: roots > stems > leaves. The metal concentrations (µg/g) in the leaves of A. viridis ranged from 0.45 to 2.18 dry weight (dw) (0.05–0.26 wet weight (ww)), 74.8 to 535 dw (8.97–64.2 ww), 2.02 to 7.45 dw (0.24–0.89 ww), and 65.2 to 521 dw (7.83–62.6 ww), for Cd, Fe, Ni, and Zn, respectively. The positive relationships between the metals, the plant parts, and the geochemical factions of their habitat topsoils indicated the potential of A. viridis as a good biomonitor of Cd, Fe, and Ni pollution. With most of the values of the bioconcentration factor (BCF) > 1.0 and the transfer factor (TF) > 1.0, A. viridis was a very promising phytoextraction agent of Ni and Zn. Additionally, with most of the values of BCF > 1.0 and TF < 1.0, A. viridis was a very promising phytostabiliser of Cd and Fe. With respect to HHR, the target hazard quotients (THQ) for Cd, Fe, Pb, and Zn in the leaves of A. viridis were all below 1.00, indicating there were no non-carcinogenic risks of the four metals to consumers, including children and adults. Nevertheless, routine monitoring of PTMs in Amaranthus farms is much needed.