Hillslopes turn precipitation into runoff and thus exert important controls on various Earth system processes. It remains difficult to collect reliable data necessary for understanding and modeling these Earth system processes in real catchments. To overcome this problem, controlled experiments are being conducted at the Landscape Evolution Observatory at Biosphere 2, The University of Arizona. Previous experiments have revealed differences in hydrological response between 2 landscapes within Landscape Evolution Observatory, even though both landscapes were designed to be identical. In an attempt to discover where the observed differences stem from, we use a fully 3‐dimensional hydrological model (CATchment HYdrology) to show the effect of soil water retention characteristics and saturated hydraulic conductivity on the hydrological response of these 2 hillslopes. We also show that soil water retention characteristics can be derived at hillslope scale from experimental observations of soil moisture and matric potential. It is found that differences in soil packing between the 2 landscapes may be responsible for the observed differences in hydrological response. This modeling study also suggests that soil water retention characteristics and saturated hydraulic conductivity have a profound effect on rainfall–runoff processes at hillslope scale and that parametrization of a single hillslope may be a promising step in modeling rainfall–runoff response in real catchments.