Rising levels of atmospheric CO2 are expected to perturb forest ecosystems, although the extent to which specific ecological interactions will be modified is unclear. This research evaluates the effects of elevated CO2 and temperature, alone and in combination, on the leaf nutritional quality of Pendunculate oak (Quercus robur L.), and the implications for herbiverous insect defoliators are discussed. A 3 °C temperature rise reduced leaf nutritional quality, by reducing foliar nitrogen concentration and increasing condensed tannin content. Doubling atmospheric CO2 temporarily increased total phenolics, but also reduced leaf toughness. The nutritional quality of the second leaf flush (lammas growth) was considerably reduced at elevated CO2. It is concluded that larval development of spring-feeding defoliators and hence adult fecundity may be adversely affected by increased temperatures.