Sites within the Pajarito Plateau have widespread, if low levels, of surface contamination. The major mechanism by which contaminants are moved and redistributed is surface runoff and associated soil erosion. To better understand the processes involved, we have been making detailed measurements of water and sediment movement at three sites across the plateau, one located in a ponderosa pine forest, one in a stable pinyon-juniper woodland, and one in a rapidly eroding pinyon-juniper woodland. For the ponderosa pine site, both surface runoff (overland flow) and subsurface runoff (interflow) are important. Overland flow can be generated by intense summer rain storms, more gentle frontal storms, or snowmelt while soils are frozen; interflow, although generated mostly by melting snow, can occur any time of the year. For the pinyon-juniper sites, the most important producer of runoff is summer thunderstorms, but at all scales snowmelt runoff can be important as well. The rapidly eroding pinyon juniper site produces more runoff than the stable pinyon-juniper site and hundreds of times more erosion than either the stable pinyon-juniper or the ponderosa site. These long-term studies are providing a better conceptual understanding of runoff and erosion on the Pajarito Plateau and other similar semiarid regions and enabling better assessments of the potential for contaminant transport in these systems.