Trichloroethylene (TCE) volatilization from leaves, trunk, and soil was measured to assess the significance of these pathways from phytoremediation sites at Travis and Fairchild Air Force Bases. Measurements were scaled temporally and spatially to estimate the annual volatilization of TCE at the Travis (0.82 ± 0.51 kg/yr) and Fairchild sites (0.014 ± 0.008 kg/yr). Volatilization was primarily through the leaf (0.34 ± 0.16 kg/yr at Travis and 0.01 ± 0.06 kg/yr at Fairchild) and soil (0.48 ± 0.36 kg/yr at Travis, 0.003 ± 0.002 kg/yr at Fairchild) pathways. The larger volatilization estimate at Travis was expected because of the site's higher TCE groundwater concentrations. Using groundwater data collected in 2004 and 2009, calculations show that over the 5 year period, 1.7 and 0.015 kg of TCE were removed each year at the Travis and Fairchild sites, respectively. On the basis of the scaled field measurements, volatilization from the leaves and soil may play a significant role in TCE removal at both sites. Daily and seasonal variations were not addressed during the limited daytime sampling events, but the methods described here provide a novel and practical framework for evaluating the potential importance of volatilization of TCE and similar compounds at phytoremediation sites. © 2013 American Chemical Society.