Improved understanding of the complex dynamics associated with spatially and temporally variable runoff response is needed to better understand the hydrology component of interdisciplinary problems. The objective of this study was to quantitatively characterize the environmental controls on runoff generation for the range of different streamflow-generation mechanisms illustrated in the classic Dunne diagram. The comprehensive physics-based model of coupled surface-subsurface flow, InHM, is employed in a heuristic mode. InHM has been employed previously to successfully simulate the observed hydrologic response at four diverse, well-characterized catchments, which provides the foundation for this study. The C3 and CB catchments are located within steep, forested terrain; the TW and R5 catchments are located in gently sloping rangeland. The InHM boundary-value problems for these four catchments provide the corner-stones for alternative simulation scenarios designed to address the question of how runoff begins (and ends). Simulated rainfall-runoff events are used to systematically explore the impact of soil-hydraulic properties and rainfall characteristics. This approach facilitates quantitative analysis of both integrated and distributed hydrologic responses at high-spatial and temporal resolution over the wide range of environmental conditions represented by the four catchments. The results from 140 unique simulation scenarios illustrate how rainfall intensity/depth, subsurface permeability contrasts, characteristic curve shapes, and topography provide important controls on the hydrologic-response dynamics. The processes by which runoff begins (and ends) are shown, in large part, to be defined by the relative rates of rainfall, infiltration, lateral flow convergence, and storage dynamics within the variably saturated soil layers.