Basin landscapes possess an identifiable spatial structure, fashioned by climate, geology and land use, that affects their hydrologic response. This structure defines a basin's hydrogeological signature and corresponding patterns of runoff and stream chemistry. Interpreting this signature expresses a fundamental understanding of basin hydrology in terms of the dominant hydrologic components: surface, interflow and groundwater runoff. Using spatial analysis techniques, spatially distributed watershed characteristics and measurements of rainfall and runoff, we present an approach for modelling basin hydrology that integrates hydrogeological interpretation and hydrologic response unit concepts, applicable to both new and existing rainfall-runoff models. The benefits of our modelling approach are a clearly defined distribution of dominant runoff form and behaviour, which is useful for interpreting functions of runoff in the recruitment and transport of sediment and other contaminants, and limited over-parameterization. Our methods are illustrated in a case study focused on four watersheds (24 to 50 km 2 ) draining the southern coast of California for the period October 1988 though to September 2002. Based on our hydrogeological interpretation, we present a new rainfall-runoff model developed to simulate both surface and subsurface runoff, where surface runoff is from either urban or rural surfaces and subsurface runoff is either interflow from steep shallow soils or groundwater from bedrock and coarse-textured fan deposits. Our assertions and model results are supported using streamflow data from seven US Geological Survey stream gauges and measured stream silica concentrations from two Santa Barbara Channel-Long Term Ecological Research Project sampling sites.