Combined sewer overflows (CSOs) discharge organic micropollutants (MPs) into open water bodies, posing potential environmental threats. Knowledge of the numbers, sources, and dynamics of MPs during CSOs is scarce but crucial for assessing their impact and developing mitigation strategies. To shed light on the dynamics of dissolved organic MPs in CSOs, we conducted high-temporal-resolution sampling (10 min composite samples) followed by liquid chromatography high-resolution mass spectrometry analysis, both target (60 substances) and nontarget, at two CSO sites in a small (17 hectares reduced (hared)) and a large (368 hared) catchment for over 10 events each. We observe similar patterns among indoor substances in the large catchment and among tire-associated compounds in both catchments, indicating source-specific behavior. Due to high and diverse concentration variability, no temporal correlations were found among indoor substances in the small catchment or among pesticides in either catchment. A random forest classifier was applied to assign nontarget time series to indoor and road sources in the large catchment. The results indicate that CSOs discharge several thousand substances from indoor sources, followed by a few hundred from outdoor sources with continuous leaching. These high numbers substantially surpass the scope of traditional target lists and underscore the importance of broad-spectrum screening methods when assessing MP contamination.