Ecological and agronomic research suggests that increased crop diversity in species-poor intensive systems may improve their provision of ecosystem services. Such general predictions can have critical importance for worldwide food production and agricultural practice but are largely untested at higher levels of diversity. 2We propose new methodology for the design and analysis of experiments to quantify diversity-function relationships. Our methodology can quantify the relative strength of inter-specific interactions that contribute to a functional response, and can disentangle the separate contributions of species richness and relative abundance. 3Applying our methodology to data from a common experiment at 28 European sites, we show that the above-ground biomass of four-species mixtures (two legumes and two grasses) in intensive grassland systems was consistently greater than that expected from monoculture performance, even at high productivity levels. The magnitude of this effect generally resulted in transgressive overyielding. 4A combined analysis of first-year results across sites showed that the additional performance of mixtures was driven by the number and strength of pairwise inter-specific interactions and the evenness of the community. In general, all pairwise interactions contributed equally to the additional performance of mixtures; the grass-grass and legume-legume interactions were as strong as those between grasses and legumes. 5The combined analysis across geographical and temporal scales in our study provides a generality of interpretation of our results that would not have been possible from individual site analyses or experimentation at a single site. 6Our four-species agricultural grassland communities have proved a simple yet relevant model system for experimentation and development of methodology in diversity-function research. Our study establishes that principles derived from biodiversity research in extensive, semi-natural grassland systems are applicable in intensively managed grasslands with agricultural plant species. ; We were supported by the EU Commission through COST Action 852. L.K. was supported by the Irish Environmental Protection Agency. It is with great regret that we note the tragic death of one of our authors, Chiara Coran. Chiara was a young and energetic member of the COST852 team. We wish to express our deep sympathy to her family and colleagues.