The status and sustainability of Poaceae crops, wheat and barley, were examined in an Atlantic zone climate. Intensification had caused yield to rise 3-fold over the last 50 years but had also degraded soil and biodiversity. Soil carbon and nitrogen were compared with current growth and yield of crops. The yield gap was estimated and options considered for raising yield. Organic carbon stores in the soil (C-soil) ranged from <2% in intensified systems growing long-season wheat to >4% in low-input, short-season barley and grass. Carbon acquisition by crops (C-crop) was driven mainly by length of season and nitrogen input. The highest C-crop was 8320 kg ha−1 C in long-season wheat supported by >250 kg ha−1 mineral N fertiliser and the lowest 1420 kg ha−1 in short-season barley fertilised by livestock grazing. Sites were quantified in terms of the ratio C-crop to C-soil, the latter estimated as the mass of carbon in the upper 0.25 m of soil. C-crop/C-soil was <1% for barley in low-input systems, indicating the potential of the region for long-term carbon sequestration. In contrast, C-crop/C-soil was >10% in high-input wheat, indicating vulnerability of the soil to continued severe annual disturbance. The yield gap between the current average and the highest attainable yield was quantified in terms of the proportion of grain sink that was unfilled. Intensification had raised yield through a 3- to 4-fold increase in grain number per unit field area, but the potential grain sink was still much higher than the current average yield. Filling the yield gap may be possible but could only be achieved with a major rise in applied nitrogen. Sustainability in Poaceae cropping now faces conflicting demands: (a) conserving and regenerating soil carbon stores in high-input systems, (b) reducing GHG emissions and other pollution from N fertiliser, (c) maintaining the yield or closing the yield gap, and (d) readjusting production among food, feed, and alcohol markets. Current cropping systems are unlikely to satisfy these demands. Transitions are needed to alternative systems based on agroecological management and biological nitrogen fixation.