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Here we tested the capacity of zero valent iron nanoparticles (nZVI) combined with two organic amendments, namely, compost and biochar, to immobilize metal(oid)s such as As, Cu, Pb, and Zn. In addition, the effects of the amendments on the development of Brassica juncea L., a plant widely used for phytoremediation purposes, were also examined. To perform the experiments, pots containing polluted soil were treated with nZVI, compost-biochar, or a blend of compost-biochar-nZVI. Metal(oid)s availability and soil properties were evaluated after 15 and 75 days, and the height and weight of the plants were measured to determine development. The compost-biochar amendment showed excellent capacity to immobilize metals, but As availability was considerably increased. However, the addition of nZVI to the mixture corrected this effect considerably. In addition, soil treatment with nZVI alone led to a slight increase in Cu availability, which was not observed for the mixture with organic amendments. With respect to soil properties, the CEC and pH were enhanced by the compost-biochar amendment, thereby favoring plant growth. Nevertheless, the nanoparticles reduced the concentration of available P, which impaired plant growth to a certain extent. In conclusion, Fe-based nanoparticles combined with organic amendments emerge as powerful approaches to remediate soils contaminated by metals and metalloids.