Healthy and tasty: these attributes define edible wild ( Diplotaxis tenuifolia) and salad rocket ( Eruca sativa), for their glucosinolate profile, that was characterised by variation in some key components. Ample variability was also detected in other Diplotaxis, with extremely glucosinolate-rich species, and strongly characterised profiles, revealing likely taxonomic affinities among taxa previously examined by other criteria, and suggesting potentials of exploitation. Leaf glucosinolates of 42 Diplotaxis and 21 Eruca accessions were studied. Total content ranged from 0.25 to more than 70 g kg −1 dry wt. The 13 clusters, defined on the basis of glucosinolate composition, belonged to two glucosinolate-rich groups, characterised by the prevalence of a single component, and one low-glucosinolate group, with a profile not dominated by any individual component. A sinigrin-rich cluster ( D. ibicensis, D. berthautii, D. ilorcitana, D. siettiana, D. tenuisiliqua, D. brevisiliqua, and D. virgata) and a gluconapin-rich cluster ( D. catholica, D.siifolia, D. virgata, and D. ollivieri) included all the species previously classified in the nigra phylogenetic lineage. D. virgata was confirmed to be a critical taxon, with one accession slightly diverging from the others. D. siifolia subsp. vicentina was separated from the others in a glucobrassicin-rich cluster. D. harra, a rather isolated representative of sub-genus Hesperidium, clustered together D. assurgens in a sinalbin-rich cluster. Another well defined cluster was represented by D. brachycarpa (gluconasturtin). The two sub-species of D. erucoides were well differentiated by their glucosinolate profile. The low glucosinolate species: D. tenuifolia, D. viminea, D. cretacea, D. muralis (subgenus Diplotaxis), and E. vesicaria, all previously included in the rapa/oleracea lineage, belonged to seven less defined clusters, mainly differing on the presence/absence or the relative abundance of some components (glucoraphanin, glucolepidin, 4-hydroxy-glucobrassicin, 4-phenylbutyl gls, glucoerucin and neoglucobrassicin). The data support previous taxonomic works. Glucosinolate-rich taxa, with well characterised profiles may be suitable for industrial uses, whereas the variability of edible D. tenuifolia and E. vesicaria may represent a basis for breeding horticultural types.