Large-scale hydrologic models are increasingly being developed for operational use in the forecasting and planning of water resources. However, the predictive strength of such models depends on how well they resolve various functions of catchment hydrology, which are influenced by gradients in climate, topography, soils, and land use. Most assessments of hydrologic model uncertainty have been limited to traditional statistical methods. Here, we present a proof-of-concept approach that uses interpretable machine learning techniques to provide post hoc assessment of model sensitivity and process deficiency in hydrologic models. We train a random forest model to predict the Kling–Gupta efficiency (KGE) of National Water Model (NWM) and National Hydrologic Model (NHM) streamflow predictions for 4383 stream gauges in the conterminous United States. Thereafter, we explain the local and global controls that 48 catchment attributes exert on KGE prediction using interpretable Shapley values. Overall, we find that soil water content is the most impactful feature controlling successful model performance, suggesting that soil water storage is difficult for hydrologic models to resolve, particularly for arid locations. We identify nonlinear thresholds beyond which predictive performance decreases for NWM and NHM. For example, soil water content less than 210 mm, precipitation less than 900 mm yr⁻¹, road density greater than 5 km km⁻², and lake area percent greater than 10 % contributed to lower KGE values. These results suggest that improvements in how these influential processes are represented could result in the largest increases in NWM and NHM predictive performance. This study demonstrates the utility of interrogating process-based models using data-driven techniques, which has broad applicability and potential for improving the next generation of large-scale hydrologic models.