This article explores a modern approach to designing carbon dioxide (СО2) sorbents based on the concept of the potential energy landscape (PEL). The authors analyze the relationship between PEL characteristics and СО2 sorption efficiency. The article demonstrates how manipulating PEL parameters enables the development of optimized materials with desired sorption properties. The article investigates the influence of the depth and distribution of energy minima on the selectivity, capacity, and kinetics of СО2 sorption. Various strategies for modifying the PEL, including surface functionalization and the targeted introduction of defects, to achieve the desired sorption characteristics are highlighted. Examples of different types of sorbents, such as MOFs, zeolites, and activated carbons, designed within the framework of the PEL concept. Potential applications of the developed sorbents in carbon capture and storage technologies, as well as the synthesis of chemically valuable products. This review will be of interest to specialists in materials science and energy who are engaged in the development of new sorption materials.