In an effort to mitigate carbon dioxide (CO2) emissions in the atmosphere, the Southeast Offshore Storage Resource Assessment (SOSRA) project has for objective to identify geological targets for CO2 storage in two main areas: the eastern part of the Gulf of Mexico and the Atlantic Ocean subsurface. SOSRA's second objective is to estimate the geological targets' capacity to store up to 30 million metric tons of CO2 each year with an error margin of ±30%. As part of this project, the research presented here focuses on the outer continental shelf of North Carolina and its potential for the deployment of large-scale offshore carbon storage in the near future. To identify geological targets, workflow followed typical early oil and gas exploration protocols: collecting existing datasets, selecting the most applicable datasets for reservoir exploration, and interpreting datasets to build a comprehensive regional geological framework of the subsurface of the outer continental shelf. The geomodel obtained can then be used to conduct static volumetric calculations estimating the storage capacity of each identified target. Numerous uncertainties regarding the geomodel were attributed to the variable coverage and quality of the geological and geophysical data. To address these uncertainties and quantify their potential impact on the storage capacity estimations, dynamic volumetric calculations (reservoir simulations) were conducted. Results have shown that, in this area, both Upper and Lower Cretaceous Formations have the potential to store large amounts of CO2 (in the gigatons range). However, sensitivity analysis highlighted the need to collect more data to refine the geomodel and thereby reduce the uncertainties related to the presence, dimensions and characteristics of potential reservoirs and seals. Reducing these uncertainties could lead to more accurate storage capacity estimations. Adequate injection strategies could then be developed based on robust knowledge of this area, thus increasing the probability of success for carbon capture and storage (CCS) offshore projects in North Carolina's outer continental shelf. / Doctor of Philosophy / Since the industrial revolution, a significant increase in the anthropogenic emissions of greenhouse gases has been observed worldwide. The rise in concentration of these gases in the atmosphere, specifically carbon dioxide (CO₂), has been linked to an increase in the average temperature on Earth, what is commonly known as global warming. To mitigate the emission of anthropogenic CO₂ in the atmosphere and consequently limit its impact on Earth’s climate, Carbon Capture and Storage projects (CCS) have been developed on various scales. In this type of project, CO₂ is captured from an emitting source (e.g., power plants), then transported via pipelines and stored in deep geological formations. In the United States, onshore CCS projects have demonstrated the technical feasibility of such projects. However, controversies associated with public acceptance and mineral ownership make expansive onshore CCS project development complicated. For these reasons, the U.S. Department of Energy (DOE) has been investigating offshore locations for the deployment of large-scale CCS projects. Southeast Offshore Storage Resource Assessment (SOSRA) is a project sponsored by the U.S. DOE to assess the storage potential of the eastern part of the Gulf of Mexico and the Atlantic Ocean as a first step towards the development of large-scale offshore storage of CO₂. The state of North Carolina was identified as an adequate candidate for CO₂ offshore storage due to its location on the Atlantic coast and its elevated CO₂ emissions from the power plants on its coastal plains. However, as exploration conducted on the outer continental shelf of North Carolina has been minimal, published information regarding the subsurface of this area remains limited to this date. To ensure the safe, long-term storage of CO₂ in this area, an extensive study was needed to select suitable geological formations and determine the storage capacity of each identified target. The research described here aimed to identify such geological targets and estimate the CO₂ storage capacity of North Carolina’s outer continental shelf