In this study, the effects of iron (Fe) nanoparticles (NPs) on Fe and heavy metal accumulations by castor (Ricinus communis L.) plants were investigated. The castor cultivar was planted in the soil contaminated with Pb and Zn for 48 days with Fe2O3 NPs treatments. The Fe and heavy metal concentrations in the plant tissues, the plant tissues' ultrastructures, and the Fe and heavy metal distributions in the soil aggregate were analyzed. The results of this study indicate that there is a mutual promotion relationship between Fe and heavy metals (Pb and Zn). The scanning electron microscopy (SEM) revealed ultrastructural differences in the xylem and phloem with Fe2O3 NPs addition, and the presence of Fe2O3 NPs may influence the synthesis of starch granules in response to heavy metal stress. Based on the analysis of the soil aggregate, α-Fe2O3 NPs and γ-Fe2O3 NPs changed the size distribution of the soil aggregate, that is, the macro-aggregate and the clay fraction contents increased and the micro-aggregate content decreased. Moreover, in the different size fractions of the soil aggregate, Fe2O3 NPs can change the Zn and Fe enrichment and migration between the macro-aggregate and clay fractions, and there is a synergistic effect between the Fe and Zn migration. In addition, in the castor organs (roots and shoots), the Zn accumulation was mainly determined by the Zn concentration of the macro-aggregate fraction, while the Fe accumulation was mainly determined by the Fe concentration of the micro-aggregate fraction. Overall, these direct observations help improve our understanding of the migration and transport characteristics of Fe and heavy metals in soil-plant systems when Fe nanoparticles are added to metal-contaminated soils.