Large-scale geological sequestration of CO2 is one of the most effective strategies to limit global warming to below 2 °C, as recommended by the Intergovernmental Panel on Climate Change (IPCC). Therefore, identifying and characterizing high-quality storage units is crucial. The Surma Basin, with its four-way dip closed structures, high-quality reservoirs, and thick regional cap rocks, is an ideal location for CO2 storage. This study focuses on the Bokabil Formation, the most prominent reservoir unit in the Surma Basin. Detailed petrographic, petrophysical, XRD, and SEM analyses, along with mapping, have been conducted to evaluate the properties of the reservoir and cap rock within this formation. The Upper Bokabil Sandstone in the Surma Basin ranges from 270 to 350 m in thickness and consists of fine- to medium-grained subarkosic sandstones composed of 70–85% quartz and 5–12% feldspar, with good pore connectivity. Petrophysical analysis of data from four gas fields indicates that this unit has a total porosity of 21–27.4% and a low shale volume of 15–27%. Cross plots and outcrop observations suggest that most of the shales are laminated within the reservoir. The regional cap rock, known as the Upper Marine Shale (UMS), ranges in thickness from 40 to 190 m and contains 10–40 nm nano-type pores. A higher proportion of ductile materials with a significant percentage of quartz in the UMS indicates higher capillary entry pressures, enhancing its capacity to hold CO2. Using the CSLF method with a 6% cut-off of the available pore volume, it is estimated that 103 Mt, 110 Mt, 205 Mt, and 164 Mt of CO2 can be effectively stored in the Sylhet, Kailashtila, Habiganj, and Fenchuganj structures, respectively. Due to the shallow depth of the storage unit and the thick cap rock, the southern Surma Basin is the optimal location for CO2 injection.