Nutrient element concentrations and grain quality were assessed in spring wheat grown under elevated CO2 concentrations and contrasting levels of tropospheric ozone at different nitrogen supply rates at several European sites. Carbon dioxide enrichment proved to affect nutrient concentrations in a complex manner. In green leaves, all elements (with exception of phosphorus and iron) decreased. In contrast, effects on the element composition of grains were restricted to reductions in nitrogen, calcium, sulphur and iron. Ozone exposure resulted in no significant effects on nutrient element concentrations in different tissues in the overall analysis. The nitrogen demand of green tissues was reduced due to CO2 enrichment as shown by reductions in the critical leaf nitrogen concentration and also enhanced nitrogen use efficiency. Reductions in the content of ribulose-bisphosphate carboxylase/oxygenase and repression of the photorespiratory pathway and reduced nitrogen allocation to enzymes driving the photosynthetic carbon oxidation cycle were chiefly responsible for this effect. Thus, nitrogen acquisition by the crop did not match carbon acquisition under CO2 enrichment. Since crop nitrogen uptake from the soil was already completed at anthesis, nitrogen allocated to the grain after anthesis originated from vegetative pools - causing grain nitrogen concentrations to decrease under CO2 enrichment (on average by 15% when CO2 concentrations increased from 360 to 680 μmol mol-1). Correspondingly, grain quality was reduced by CO2 enrichment. The Zeleny value, Hagberg value and dry/wet gluten content decreased significantly with increasing [CO2]. Despite the beneficial impact of CO2 enrichment on growth and yield of C3 cereal crops, declines in flour quality due to reduced nitrogen content are likely in a future, [CO2]-rich world.