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Abstract Understanding controls on solute export to streams is challenging because heterogeneous catchments can respond uniquely to drivers of environmental change. To understand general solute export patterns, we used a large‐scale inductive approach to evaluate concentration–discharge (C–Q) metrics across catchments spanning a broad range of catchment attributes and hydroclimatic drivers. We leveraged paired C–Q data for 11 solutes from CAMELS‐Chem, a database built upon an existing dataset of catchment and hydroclimatic attributes from relatively undisturbed catchments across the contiguous USA. Because C–Q relationships with Q thresholds reflect a shift in solute export dynamics and are poorly characterized across solutes and diverse catchments, we analysed C–Q relationships using Bayesian segmented regression to quantify Q thresholds in the C–Q relationship. Threshold responses were rare, representing only 12% of C–Q relationships, 56% of which occurred for solutes predominantly sourced from bedrock. Further, solutes were dominated by one or two C–Q patterns that reflected vertical solute–source distributions. Specifically, solutes predominantly sourced from bedrock had diluting C–Q responses in 43%–70% of catchments, and solutes predominantly sourced from soils had more enrichment responses in 35%–51% of catchments. We also linked C–Q relationships to catchment and hydroclimatic attributes to understand controls on export patterns. The relationships were generally weak despite the diversity of solutes and attribute types considered. However, catchment and hydroclimatic attributes in the central USA typically drove the most divergent export behaviour for solutes. Further, we illustrate how our inductive approach generated new hypotheses that can be tested at discrete, representative catchments using deductive approaches to better understand the processes underlying solute export patterns. Finally, given these long‐term C–Q relationships are from minimally disturbed catchments, our findings can be used as benchmarks for change in more disturbed catchments. 

Abstract. Large sample datasets are transforming the catchment sciences, but there are few off-the-shelf stream water chemistry datasets with complementary atmospheric deposition, streamflow, meteorology, and catchment physiographic attributes. The existing CAMELS (Catchment Attributes and Meteorology for Large-sample Studies) dataset includes data on topography, climate, streamflow, land cover, soil, and geology across the continental US. With CAMELS-Chem, we pair these existing attribute data for 516 catchments with atmospheric deposition data from the National Atmospheric Deposition Program and water chemistry and instantaneous discharge data from the US Geological Survey over the period from 1980 through 2018 in a relational database and corresponding dataset. The data include 18 common stream water chemistry constituents: Al, Ca, Cl, dissolved organic carbon, total organic carbon, HCO3, K, Mg, Na, total dissolved N, total organic N, NO3, dissolved oxygen, pH (field and lab), Si, SO4, and water temperature. Annual deposition loads and concentrations include hydrogen, NH4, NO3, total inorganic N, Cl, SO4, Ca, K, Mg, and Na. We demonstrate that CAMELS-Chem water chemistry data are sampled effectively across climates, seasons, and discharges for trend analysis and highlight the coincident sampling of stream constituents for process-based understanding. To motivate their use by the larger scientific community across a variety of disciplines, we show examples of how these publicly available datasets can be applied to trend detection and attribution, biogeochemical process understanding, and new hypothesis generation via data-driven techniques.