Book excerpt: Diffusive transport of volatile organic compounds (VOCs) and their degradation by bacteria in unsaturated soils are coupled by poorly understood mass transfer kinetics at the gas/water interface. The capability to predict the fate of VOCs in m saturated soil is necessary to evaluate the feasibility of natural attenuation as a VOC remediation strategy. The objective of this study was to develop a mechanistically based mathematical model that considered the interdependence of VOC diffusive transport, mass transfer at the gas/water interface, microbial activity, and sorptive interactions in a moist, unsaturated soil. Because the focus of the model was on description of natural attenuation, the advective VOC transport that is induced in engineered remediation processes such as vapor extraction was not considered. The utility of the model was assessed through its ability to describe experimental observations from well-defined experiments in which toluene was used as a representative VOC and diffused through soil columns that contained a toluene degrading bacterium, Pseudomonasputida. The coefficient for gas-liquid mass-transfer, KLa, was found to be a key parameter controlling the ability of bacteria to degrade VOCs. This finding indicates that soil size and geometry are likely to be dominant parameters in assessing the possible success of natural attenuation of VOCs in contaminated unsaturated soils.