A significant fraction of Earth consists of mountainous terrain. However, the question of how to monitor the surface–atmosphere carbon exchange over complex terrain has not been fully explored. This article reports on studies by a team of investigators from U.S. universities and research institutes who carried out a multiscale and multidisciplinary field and modeling investigation of the CO2exchange between ecosystems and the atmosphere and of CO2 transport over complex mountainous terrain in the Rocky Mountain region of Colorado. The goals of the field campaign, which included ground and airborne in situ and remote-sensing measurements, were to characterize unique features of the local CO2 exchange and to find effective methods to measure regional ecosystem–atmosphere CO2exchange over complex terrain. The modeling effort included atmospheric and ecological numerical modeling and data assimilation to investigate regional CO2 transport and biological processes involved in ecosystem-atmosphere carbon exchange. In this report, we document our approaches, demonstrate some preliminary results, and discuss principal patterns and conclusions concerning ecosystem-atmosphere carbon exchange over complex terrain and its relation to past studies that have considered these processes over much simpler terrain.