Prominent among the many factors now affecting the sustainability of forest ecosystems are anthropogenically-generated carbon dioxide (CO2) and ozone (O3). CO2 is the substrate for photosynthesis and thus can accelerate tree growth, whereas O3 is a highly reactive oxygen species and interferes with basic physiological functions. This review summarizes the impacts of CO2 and O3 on tree chemical composition and highlights the consequences thereof for trophic interactions and ecosystem dynamics. CO2 and O3 influence phytochemical composition by altering substrate availability and biochemical/physiological processes such as photosynthesis and defense signaling pathways. Growth of trees under enriched CO2 generally leads to an increase in the C/N ratio, due to a decline in foliar nitrogen and concomitant increases in carbohydrates and phenolics. Terpenoid levels generally are not affected by atmospheric CO2 concentration. O3 triggers up-regulation of antioxidant defense pathways, leading to the production of simple phenolics and flavonoids (more so in angiosperms than gymnosperms). Tannins levels generally are unaffected, while terpenoids exhibit variable responses. In combination, CO2 and O3 exert both additive and interactive effects on tree chemical composition. CO2-and O3-mediated changes in plant chemistry influence host selection, individual performance (development, growth, reproduction), and population densities of herbivores (primarily phytophagous insects) and soil invertebrates. These changes can effect shifts in the amount and temporal pattern of forest canopy damage and organic substrate deposition. Decomposition rates of leaf litter produced under elevated CO2 and O3 may or may not be altered, and can respond to both the independent and interactive effects of the pollutants. Overall, however, CO2 and O3 effects on decomposition will be influenced more by their impacts on the quantity, rather than quality, of litter produced. A prominent theme to emerge from this and related reviews is that the effects of elevated CO2 and O3 on plant chemistry and ecological interactions are highly context- and species-specific, thus frustrating attempts to identify general, global patterns. Many of the interactions that govern above- and below-ground community and ecosystem processes are chemically mediated, ultimately influencing terrestrial carbon sequestration and feeding back to influence atmospheric composition. Thus, the discipline of chemical ecology is fundamentally important for elucidating the impacts of humans on the health and sustainability of forest ecosystems. Future research should seek to increase the diversity of natural products, species, and biomes studied; incorporate long-term, multi-factor experiments; and employ a comprehensive “genes to ecosystems” perspective that couples genetic/genomic tools with the approaches of evolutionary and ecosystem ecology.