Ecological studies identifying a positive relationship between biodiversity and ecosystem services motivate projections that higher plant diversity will increase services from agroecosystems. While this idea is compelling, evidence of generalizable relationships between biodiversity and ecosystem services that could be broadly applied in agricultural systems is lacking. Cover crops grown in rotation with cash crops are a realistic strategy to increase agroecosystem diversity. We evaluated the prediction that further increasing diversity with cover crop polycultures would enhance ecosystem services and multifunctionality in a 2-year study of eighteen cover crop treatments ranging in diversity from one to eight species. Five ecosystem services were measured in each cover crop system and regression analysis used to explore the relationship between multifunctionality and several diversity indices.