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Improving iron (Fe) concentration in staple grain crops could help reduce Fe-deficiency anaemia in communities dependent on plant-based diets. Co-application of nitrogen (N) and zinc (Zn) fertilizers has been reported to improve both yield and grain Zn concentration of crops in smallholder farming systems. This study was conducted to determine if similar effects are observed for grain Fe concentration. Field experiments were conducted in two years, in two contrasting agro-ecologies in Zimbabwe, on maize (Zea mays L.), cowpea (Vigna unguiculata [L.] Walp) and two finger millet (Eleusine coracana (L.) Gaertn.) “seed pools”. The two finger millet “seed pools” were collected during previous farmer surveys to represent “high” and “low” Fe concentrations. All plots received foliar Fe-ethylene diamine tetra-acetic acid (EDTA) fertilizer and one of seven N treatments, representing mineral or organic N sources, and combinations thereof. Higher grain yields were observed in larger N treatments. Grain Fe concentration increased according to species: maize < finger millet < cowpea but varied widely according to treatment. Significant effects of N-form on grain Fe concentration were observed in the low finger millet “seed pool”, for which mineral N fertilizer application increased grain Fe concentration to a greater extent than other N forms, but not for the other species. Whilst good soil fertility management is essential for yield and grain quality, effects on grain Fe concentration are less consistent than reported previously for Zn.