The flux of volatile organic chemicals from natural vegetation influences various atmospheric properties including oxidation state of the troposphere via the hydroxyl radical (OH), photochemical haze production and the concentration of greenhouse gases (CH4, H2O, CO). Because the Volatile Organic Compound (VOC) flux in the present-day world varies markedly with both vegetation cover and with climate, changes in the emission of VOCs may have damped or amplified past climate changes. Here we conduct a preliminary study on possible changes in VOC emission resulting from broad scale vegetation and climate change since the Last Glacial Maximum (LGM). During the general period of the LGM (~25-17,000 years before present {BP}), global forest cover was considerably less than in the present potential situation. The change in vegetation would have resulted in a ~30% reduction in VOC emission at 643 Tg y-1 relative to the present potential vegetation (912.9 Tg y-1). Uncertainty in global vegetation cover during the LGM bounds the VOC estimate by ±15%. In contrast, during the warmer early-to-mid Holocene (8000 and 5000 BP), with greater forest extent and less desert than during the late Holocene (0 BP), emission rates of VOCs seem likely to have been higher than at present. Further modifications in VOC emission may have been mediated by a reduction in mean tropical lowland temperatures (by around 5-6°C) decreasing the LGM VOC emission estimate by 38% relative to the warmer LGM scenario. Increased VOC emissions due to forest expansion and increased tropical temperatures since the LGM may have served as a significant driver of climate change over the last 15 ka y through the influence of VOC oxidation; this can impact tropospheric radiative balance through reductions in the concentration of OH, increasing the concentration of CH4. The error limits on past VOC emission estimates are large, given the uncertainties of present-day VOC emission rates, paleoecosystem distribution, tropical paleoclimatic conditions, and physiological assumptions regarding controls over VOC emission. Nevertheless, the potential significance of changes in natural VOC emission over the last 20 ka and their influence on climate are an important unknown that should at least be borne in mind as a limit on the understanding of past atmospheric conditions. Elucidation of the role of VOCs in climate change through paleoclimatic general circulation model simulations may improve understanding of past and future changes in climate. (C) 2000 Elsevier Science Ltd.