Although carbon capture, utilization, and storage (CCUS) has enormous emission reduction potential and application prospects, it still faces many obstacles and challenges in the actual deployment and promotion process. This study aims to evaluate the spatial suitability of the CCUS layout comprehensively and deeply analyze key development obstacles to provide a scientific basis for the promotion and layout of CCUS. Therefore, this article constructs a combination of Geographic Information Systems (GIS), Decision-making trial and evaluation laboratory (DEMATEL) method, and Interpretive structure model (ISM). Firstly, a comprehensive evaluation is conducted on the suitability of the CCUS layout in China based on GIS technology, identifying high-potential areas. The results indicate that when the threshold is 80% of the highest score for suitability, a total area of 1.46 million square kilometers is suitable for the CCUS project layout. When it dropped to 60%, this data increased to 2.04 million square kilometers. These areas are mainly distributed in large basin areas with abundant resources. Secondly, the DEMATEL-ISM analysis framework is improved to systematically identify and analyze the key obstacles that constrain the promotion of CCUS in China. The results indicate that there is a very complex relationship between the obstacles that constrain the development of CCUS, with the fundamental reasons being the lagging technological level and imperfect policies and regulations. Finally, goal-oriented suggestions and response measures were proposed, and targeted analysis was conducted on high-suitability areas. This study constructed an interdisciplinary methodology interpretive model to provide decision support for the CCUS layout and targeted strategies to break through current development barriers and promote the rapid development of CCUS.