Global food security in a changing climate depends on both the nutritive value of staple crops as well as their yields. Here, we examined the direct effect of atmospheric carbon dioxide on the toxicity of the important pasture crop, Trifolium repens L. (clover). Shoots of T. repens contain cyanogenic glycosides that break down to release toxic hydrogen cyanide when damaged. The ability of animals to tolerate cyanogenic compounds is dependent, in part, on their overall protein intake. We grew T. repens communities at ambient and approximately twice-ambient CO2 in a controlled environment greenhouse experiment. We found that the ratio of total cyanogenic glycosides to total protein ratio was nearly two times higher in leaves of T. repens grown at elevated CO2. This study highlights the importance of assessing the nutritive value of this and other plants in response to rising CO2 so that steps can be taken to address any adverse consequences for herbivores.