Bioenergy is expected to play an increasingly significant role in the global energy budget. In addition to the use of liquid energy forms such as ethanol and biodiesel, electricity generation using processed energy crops as a partial or full coal alternative is expected to increase, requiring large-scale conversions of land for the cultivation of bioenergy feedstocks such as cane, grasses, or short rotation coppice. With land-use change identified as a major contributor to changes in the emission of biogenic volatile organic compounds (BVOCs), many of which are known contributors to the pollutants ozone (O3) and fine particulate matter (PM2.5), careful review of crop emission profiles and local atmospheric chemistry will be necessary to mitigate any unintended air-quality consequences. In this work, the atmospheric consequences of bioenergy crop replacement are examined using both the high-resolution regional chemical transport model WRF/Chem (Weather Research and Forecasting with Chemistry) and the global climate model CESM (Community Earth System Model). Regional sensitivities to several representative crop types are analyzed, and the impacts of each crop on air quality and climate are compared. Overall, the high emitting crops (eucalyptus and giant reed) were found to produce climate and human health costs totaling up to 40% of the value of CO2 emissions prevented, while the related costs of the lowest-emitting crop (switchgrass) were negligible.