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In dry summer months, stream baseflow sourced from groundwater is essential to support aquatic ecosystems and anthropogenic water use. Hydrologic signatures, or metrics describing unique features of streamflow timeseries, are useful for quantifying and predicting these valuable baseflow and groundwater storage resources across continental scales. Hydrologic signatures can be predicted based on catchment attributes summarising climate and landscape and can be used to characterise baseflow and groundwater processes that cannot be directly measured. While past watershed‐scale studies suggest that landscape attributes are important controls on baseflow and storage processes, recent regional‐to‐global scale modelling studies have instead found that landscape attributes have weaker relationships with hydrologic signatures of these processes than expected compared to climate attributes. In this study, we quantify two landscape attributes, average geologic age and the proportion of catchment area covered by wetlands. We investigate if incorporating these additional predictors into existing large‐sample attribute datasets strengthens continental‐scale, empirical relationships between landscape attributes and hydrologic signatures. We quantify 14 hydrologic signatures related to baseflow and groundwater processes in catchments across the contiguous United States, evaluate the relationships between the new catchment attributes and hydrologic signatures with correlation analysis and use the new attributes to predict hydrologic signatures with random forest models. We found that the average geologic age of catchments was a highly influential predictor of hydrologic signatures, especially for signatures describing baseflow magnitude in catchments, and had greater importance than existing attributes of the subsurface. In contrast, we found that the proportion of wetlands in catchments had limited influence on our hydrologic signature predictions. We recommend incorporating catchment geologic age into large‐sample catchment datasets to improve predictions of baseflow and storage hydrologic signatures and processes across continental scales.