Free-air CO 2 enrichment (FACE) experiments have provided novel insights into the ecological mechanisms controlling the cycling and storage of carbon in terrestrial ecosystems and contribute to our ability to project how ecosystems respond to increasing CO 2 in the Earth's atmosphere. Important lessons emerge by evaluating a set of hypotheses that initially guided the design and longevity of forested FACE experiments. Net primary productivity is increased by elevated CO 2 , but the response can diminish over time. Carbon accumulation is driven by the distribution of carbon among plant and soil components with differing turnover rates and by interactions between the carbon and nitrogen cycles. Plant community structure may change, but elevated CO 2 has only minor effects on microbial community structure. FACE results provide a strong foundation for next-generation experiments in unexplored ecosystems and inform coupled climate-biogeochemical models of the ecological mechanisms controlling ecosystem response to the rising atmospheric CO 2 concentration.