Future progress on the creation of wheat cultivars with high grain zinc (Zn) and iron (Fe) mineral density will depend on both the availability of suitable donor germplasm and the identification of genes or quantitative trait loci contributing to increase the accumulation of mineral elements in the wheat kernels. Multi-environment field trials were conducted to evaluate the grain Zn, Fe and protein concentration of 32 bread wheat (Triticum aestivum L.) and 20 durum wheat (T. turgidum L. var. durum) landraces locally adapted to soils covering a wide range of pH values and mineral composition. These landraces were selected after a preliminary, small-scale field trial that had analysed 425 Spanish local varieties. Analyses of variance demonstrated a significant effect of genotype on grain composition, and 16 wheat landraces with elevated grain Zn and/or Fe density across the environments were identified. These landraces rich in grain minerals represent valuable primary gene-pool parents for wheat biofortification. No pattern of native soil geochemical characteristics that could help to predict the success in collecting mineral-dense genotypes in a given area was found. Mapping populations derived from some pairs of grain-mineral-rich and -poor genotypes characterised in the study may facilitate the development of molecular markers to assist the selection of superior wheat genotypes.