Cheatgrass (Bromus tectorum) is a recognized, invasive annual weed of the western United States that reduces fire return times from decades to less than 5 years. To determine the interaction between rising carbon dioxide concentration ([CO2]) and fuel load, we characterized potential changes in biomass accumulation, C : N ratio and digestibility of three cheatgrass populations from different elevations to recent and near-term projections in atmospheric [CO2]. The experimental CO2 values (270, 320, 370, 420 μmol mol−1) corresponded roughly to the CO2 concentrations that existed at the beginning of the 19th century, that during the 1960s, the current [CO2], and the near-term [CO2] projection for 2020, respectively. From 25 until 87 days after sowing (DAS), aboveground biomass for these different populations increased 1.5–2.7 g per plant for every 10 μmol mol−1 increase above the 270 μmol mol−1 preindustrial baseline. CO2 sensitivity among populations varied with elevational origin with populations from the lowest elevation showing the greatest productivity. Among all populations, the undigestible portion of aboveground plant material (acid detergent fiber ADF, mostly cellulose and lignin) increased with increasing [CO2]. In addition, the ratio of C : N increased with leaf age, with [CO2] and was highest for the lower elevational population. These CO2-induced qualitative changes could, in turn, result in potential decreases in herbivory and decomposition with subsequent effects on the aboveground retention of cheatgrass biomass. Overall, these data suggest that increasing atmospheric [CO2] above preambient levels may have contributed significantly to cheatgrass productivity and fuel load with subsequent effects on fire frequency and intensity.