Quantifying the relationships between plant functional traits and ecosystem services has been promoted as an approach to achieving multifunctional grassland systems that balance productivity with other regulating, supporting and cultural services. Establishing trade-offs and synergies between traits and services has largely relied on meta-analyses of studies from different systems and environments. This study demonstrated the value of focused studies of long-term experiments in grassland systems that measure traits and services in the same space and time to better understand the ecological constraints underlying these trade-offs and synergies. An analysis is presented that uses data from the Park Grass Experiment at Rothamsted Research on above-ground productivity, species richness and soil organic carbon stocks to quantify the relationships between these three outcomes and the power of variance in plant functional traits in explaining them. There was a trade-off between plots with high productivity, nitrogen inputs and soil organic carbon and plots with high species richness that was explained by a functional gradient of traits that are indicative of contrasting strategies of resource acquisition of resource conservation. Examples were identified of using functional traits to identify opportunities for mitigating these trade-offs and moving toward more multifunctional systems.