SUMMARYLegumes represent an important component of human and livestock diets; they are rich in macro‐ and micronutrients such as proteins, dietary fibers and polyunsaturated fatty acids. Whilst several health‐promoting and anti‐nutritional properties have been associated with grain content, in‐depth metabolomics characterization of major legume species remains elusive. In this article, we used both gas chromatography–mass spectrometry (GC‐MS) and liquid chromatography–mass spectrometry (LC‐MS) to assess the metabolic diversity in the five legume species commonly grown in Europe, including common bean (Phaseolus vulgaris), chickpea (Cicer arietinum), lentil (Lens culinaris), white lupin (Lupinus albus) and pearl lupin (Lupinus mutabilis), at the tissue level. We were able to detect and quantify over 3400 metabolites covering major nutritional and anti‐nutritional compounds. Specifically, the metabolomics atlas includes 224 derivatized metabolites, 2283 specialized metabolites and 923 lipids. The data generated here will serve the community as a basis for future integration to metabolomics‐assisted crop breeding and facilitate metabolite‐based genome‐wide association studies to dissect the genetic and biochemical bases of metabolism in legume species.