Mountain watersheds recently burned by wildfire often experience greater amounts of runoff and increased rates of sediment transport relative to similar unburned areas. Given the sedimentation and debris flow threats caused by increases in erosion, more work is needed to better understand the physical mechanisms responsible for the observed increase in sediment transport in burned environments and the time scale over which a heightened geomorphic response can be expected. In this study, we quantified the relative importance of different hillslope erosion mechanisms during two postwildfire rainstorms at a drainage basin in Southern California by combining terrestrial laser scanner-derived maps of topographic change, field measurements, and numerical modeling of overland flow and sediment transport. Numerous debris flows were initiated by runoff at our study area during a long-duration storm of relatively modest intensity. Despite the presence of a well-developed rill network, numerical model results suggest that the majority of eroded hillslope sediment during this long-duration rainstorm was transported by raindrop-induced sediment transport processes, highlighting the importance of raindrop-driven processes in supplying channels with potential debris flow material. We also used the numerical model to explore relationships between postwildfire storm characteristics, vegetation cover, soil infiltration capacity, and the total volume of eroded sediment from a synthetic hillslope for different end-member erosion regimes. This study adds to our understanding of sediment transport in steep, postwildfire landscapes and shows how data from field monitoring can be combined with numerical modeling of sediment transport to isolate the processes leading to increased erosion in burned areas.