AbstractLeakage from geologic CO2sequestration (GCS) reservoirs to overlying underground sources of drinking water (USDW) is a tangible risk. This study is an integrated assessment that combines column experiments and reactive transport simulations of sediments sampled from the Ogallala aquifer above an active commercial‐scale GCS site (the Farnsworth Unit in northern Texas). Experimental and simulation results suggest that carbonate mineral (calcite and dolomite) dissolution is the most significant reaction following CO2intrusion, and is also the dominant source of trace metal release. Cation exchange is another key mechanism controlling trace metal release by cation interference. Most of the trace metals, including Ba, Sr, As, Pb, and Zn, show a short‐term release and quickly drop to the baseline values, suggesting low risk to the overlying USDW quality. Other trace metals, such as Mn and U, exhibit a tangible increase of their concentrations in the beginning, and drop to a higher level compared to the baseline, which may become a potential concern of long‐term USDW quality change with CO2introduction. This study provides a comprehensive example of combining laboratory experiments and simulations for assessment of CO2‐sediment interactions with combined release mechanisms in shallow groundwater aquifers. Data presented here provides useful insights for quantitative risk assessment and effective public education regarding CO2geological sequestration, and trace metal reactive transport studies in shallow groundwater aquifers.