Roadway deicing agents, including rock salt and brine containing NaCl, have had a profound impact on the water quality and aquatic health of rivers and streams in urbanized areas with temperate climates. Yet, few studies evaluate impacts to watersheds characterized by relatively low impervious surface cover (ISC; < 15 %). Here, we use long-term (1997-2019), monthly streamwater quality data combined with daily streamflow for six exurban and suburban watersheds in southeastern Pennsylvania to examine the relations among chloride (Cl⁻) concentrations and ISC. Both flow-normalized Cl⁻ concentrations and ISC increased over time in each of the six watersheds, consistent with changes in watershed management (e.g., ISC, road salt application, etc.). The watersheds that experienced the greatest changes in percent ISC (e.g., agriculture replaced by residential and commercial development) experienced the greatest changes in flow-normalized Cl⁻ concentrations. We also utilized a comprehensive mass-balance model (2011–2018) that indicated Cl⁻ inputs exceeded the outputs for the study watersheds. Road salt applied to state roads, non-state roads, and other impervious surfaces accounted for the majority of Cl⁻ inputs to the six watersheds. Furthermore, increasing Cl⁻ concentrations during baseflow conditions confirm impacts to shallow groundwater. Although flow-normalized Cl⁻ concentrations are below the U.S. Environmental Protection Agency's chronic threshold value for impacts to aquatic organisms, year-round exceedances may result before the end of this century based on current trends. Though reduced Cl⁻ loading to streams may be achieved by limiting the expansion of impervious surfaces in exurban and suburban watersheds, changes in baseflow concentrations are likely to be gradual because of the accumulated Cl⁻ in groundwater.