When urbanization occurs, the removal of vegetation, compaction of soil and construction of impervious surfaces—roofs, asphalt, and concrete—and drainage infrastructure result in drastic changes to the natural hydrological cycle. Stormwater runoff occurs when rain does not infiltrate into soil. Instead it ponds at the surface and forms shallow channels of overland flow. The result is increased peak flows and pollutant loads, eroded streambanks, and decreased biodiversity in aquatic habitat. In urban areas, runoff is typically directed into catch basins and underground pipe systems to prevent flooding, however such systems are also failing to meet modern environmental goals. Green infrastructure is the widely evocative idea that development practices and stormwater management infrastructure can do better to mimic the natural hydrological conditions through distributed vegetation and source control measures that prevent runoff from being produced in the first place. This dissertation uses statistics and high-resolution, coupled surface-subsurface hydrologic simulation (ParFlow.CLM) to examine three understudied aspects of green infrastructure planning. First, I examine how development characteristics affect the runoff response in urban catchments. I find that instead of focusing on site imperviousness, planners should aim to preserve the ecosystem functions of infiltration and evapotranspiration that are lost even with low density development. Second, I look at how the spatial configuration of green infrastructure at the neighborhood scale affects runoff generation. While spatial configuration of green infrastructure does result in statistically significant differences in performance, such differences are not likely to be detectable above noise levels present in empirical monitoring data. In this study, there was no evidence of reduced hydrological effectiveness for green infrastructure located at sag points in the topography. Lastly, using six years of empirical data from a voluntary residential green infrastructure program, I show how the spread of green infrastructure depends on the demographic and physical characteristics of neighborhoods as well as spatially-dependent social processes (such as the spread of information). This dissertation advances the science of green infrastructure planning at multiple scales and in multiple sectors to improve the practice of urban water resource management and sustainable development.