The Mount Simon Sandstone and Eau Claire Formation represent a potential reservoir-caprock system for wastewater disposal, geologic CO2 storage, and compressed air energy storage (CAES) in the Midwestern United States. A primary concern to site performance is heterogeneity in rock properties that could lead to nonideal injectivity and distribution of injected fluids (e.g., poor sweep efficiency). Using core samples from the Dallas Center domal structure, Iowa, we investigate pore characteristics that govern flow properties of major lithofacies of these formations. Methods include gas porosimetry and permeametry, mercury intrusion porosimetry, thin section petrography, and X-ray diffraction. The lithofacies exhibit highly variable intraformational and interformational distributions of pore throat and body sizes. Based on pore-throat size, there are four distinct sample groups. Micropore-throat–dominated samples are from the Eau Claire Formation, whereas the macropore-dominated, mesopore-dominated, and uniform-dominated samples are from the Mount Simon Sandstone. Complex paragenesis governs the high degree of pore and pore-throat size heterogeneity, due to an interplay of precipitation, nonuniform compaction, and later dissolution of cements. The cement dissolution event probably accounts for much of the current porosity in the unit. Mercury intrusion porosimetry data demonstrate that the heterogeneous nature of the pore networks in the Mount Simon Sandstone results in a greater than normal opportunity for reservoir capillary trapping of nonwetting fluids, as quantified by CO2 and air column heights that vary over three orders of magnitude, which should be taken into account when assessing the potential of the reservoir-caprock system for waste disposal (CO2 or produced water) and resource storage (natural gas and compressed air). Our study quantitatively demonstrates the significant impact of millimeter-scale to micron-scale porosity heterogeneity on flow and transport in reservoir sandstones.