In this article's companion paper, flexible approaches for conceptual hydrological modeling at the catchment scale were motivated, and the SUPERFLEX framework, based on generic model components, was introduced. In this article, the SUPERFLEX framework and the “fixed structure” GR4H model (an hourly version of the popular GR4J model) are applied to four hydrologically distinct experimental catchments in Europe and New Zealand. The estimated models are scrutinized using several diagnostic measures, ranging from statistical metrics, such as the statistical reliability and precision of the predictive distribution of streamflow, to more process-oriented diagnostics based on flow-duration curves and the correspondence between model states and groundwater piezometers. Model performance was clearly catchment specific, with a single fixed structure unable to accommodate intercatchment differences in hydrological behavior, including seasonality and thresholds. This highlights an important limitation of any “fixed” model structure. In the experimental catchments, the ability of competing model hypotheses to reproduce hydrological signatures of interest could be interpreted on the basis of independent fieldwork insights. The potential of flexible frameworks such as SUPERFLEX is then examined with respect to systematic and stringent hypothesis-testing in hydrological modeling, for characterizing catchment diversity, and, more generally, for aiding progress toward a more unified formulation of hydrological theory at the catchment scale. When interpreted in physical process-oriented terms, the flexible approach can also serve as a language for dialogue between modeler and experimentalist, facilitating the understanding, representation, and interpretation of catchment behavior.