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We used three-dimensional (3D), high-resolution simulations facilitated by parallel computation to assess the effect of hydrogeological heterogeneity in the Mt. Simon Sandstone on CO₂ plume evolution and storage and geochemical reactions in a portion of the Illinois Basin, Indiana. Two scenarios were selected to investigate the effects of the hydrogeological heterogeneity in 3D reactive transport simulations: a heterogeneous case with variable porosity and permeability, and a homogenous case with constant porosity and permeability. The initial pressure, temperature, and mineralogical distributions are consistently applied in both the heterogeneous case and the homogeneous case. Results indicate that including hydrogeological heterogeneity in 3D reservoir simulations for geological CO₂ storage significantly impacts modeling results for plume migration patterns, CO₂-water-mineral interaction, reservoir quality, and CO₂ plume containment. In particular, results indicate that (1) the CO₂ plume reached the top of the Mt. Simon Sandstone in the homogeneous case, but was restrained to the lower third of the formation when hydrogeologic heterogeneity was considered; (2) the dominant trapping mechanism in the heterogeneous case was mineral trapping (43%), while it was solubility trapping (47%) in the homogeneous case (at 10,000 years); (3) incorporating reservoir heterogeneity in the model leads to a higher likelihood of long-term containment.