Cover crops grown in rotation with cash crops provide ecosystem services by reducing pollution and anthropogenic inputs. Among cover crop families, crucifers can efficiently prevent nitrate and sulphate leaching by catching residual soil mineral nitrogen (N) and sulphur (S) (N and S catch crop services). Crucifers also have a unique capacity to suppress pathogens due to the biocidal hydrolysis products of endogenous secondary metabolites called glucosinolates (GSL). However, compared to legume cover crops, crucifers provide less mineralised N to the subsequent main cash crop (N green manure service). Bispecific crucifer–legume cover crop mixtures can be seen as a potential solution to increase biodiversity and to combine ecosystem services of both species. However there is a lack of information on the impact of plant–plant interaction on levels of ecosystem services linked to the N and S cycles and GSL production compared to sole crops. The aim of our study was to assess production of all these ecosystem services for a wide range of bispecific crucifer-legume mixtures in comparison to sole crops. Experiments were conducted at two sites (near Toulouse and Orléans, France) over two years where few cultivars from eight crucifers (rape, white mustard, Indian mustard, Ethiopian mustard, turnip, turnip rape, radish and rocket) and nine legumes (Egyptian clover, crimson clover, common vetch, purple vetch, hairy vetch, pea, soya bean, faba bean, and white lupin) were tested in sole-crop and in 98 bispecific mixtures (substitutive design of 50%-50% sole crops). Crucifer - legume bispecific mixtures provided the same N and S catch crop service (mean soil acquisition of 50 kg N ha-1 and 12 kg S ha-1) and significantly increased the N green manure service (mean mineralisation of 22 kg N ha-1) compared to pure crucifers (mean mineralisation of 8 kg N ha-1). Despite half the density of crucifers, S green manure service was only reduced by 15% in the mixture (mean mineralisation o