Biogenic volatile organic compounds (BVOCs) play critical roles in ecological and earth-system processes.Ecosystem BVOC models rarely include soil and litter fluxes and their accuracy is often challenged by BVOC dynamics during periods of rapid ecosystem change. We measured BVOC concentrations within a mixed deciduous forest and used a hybrid Lagrangian/Eulerian canopy transport model to estimate BVOC flux from the forest floor, canopy, and whole ecosystem during spring leaf-out. Canopy flux measurements were dominated by a large methanol source and small isoprene source during the leaf-out period, consistent with past measurements and theory, and indicative of a BVOC flux situation rarely used in emissions model testing. Measurements also revealed that the contribution of the forest floor to whole-ecosystem BVOC flux is conditional on the compound of interest and often non-trivial. We then created linear models of forest floor, canopy, and whole-ecosystem flux for each study compound and used information criteriabased model selection to find the simplest model with the best fit. Vapor pressure deficit (VPD) was included in the best canopy, forest floor, and whole-ecosystem BVOC flux model more than any other study variable, but most published BVOC flux models do not include VPD. Future studies should investigate how VPD contributes to BVOC flux through biophysical mechanisms like evaporative demand, leaf temperature and stomatal function.