Iron (Fe) is an essential element for human nutrition, and its deficiency or low hemoglobin levels are a global health issue. Strategies aimed at increasing the amounts of essential elementals in agricultural products, as sprouts of adzuki bean (Vigna angularis), can be a way to minimize deficiencies, mainly in the populations of developing countries. Therefore, in this work was evaluated: production of Fe-enriched adzuki bean sprouts; Fe accumulation and translocation in plants in different culture media enriched with different Fe masses (500, 1000, 2000, and 3000 µg); and effects of the enrichment by means of 3000 µg FeIII-ethylenediaminetetraacetic acid (FeIII-EDTA): on the distribution of Ca, Cu, Fe, K, P, Mg, S, and Zn in different parts of the plant; on protein concentrations (albumins, globulins, prolamins, and glutelins) and their association with Fe in edible parts of the plant (stems); and on Fe bioaccessibility in the edible part of the plant (stems). The enrichment via FeIII-EDTA favored the translocation and increased Fe content of sprouts (75%), besides promoting interactions of Fe with albumins (141%), globulins (180%), and glutelins (93%). In the bioaccessibility assays, Fe was 83% bioaccessible in Fe-enriched sprouts.