The commercially available activated carbon was modified using barrier and spark discharge low-temperature nitrogen plasma treatment. The samples were investigated using nitrogen sorption at a temperature of −196 °C, XRD, SEM, and FTIR methods, and elemental analysis. The nitrogen content on the surface was increased, but other properties, such as specific surface area, total pore volume, pseudocrystallite height, and pseudocrystallite width, remained unchanged. The activated carbons after nitrogen plasma treatment indicated higher CO2 adsorption than the pristine ones. Since the investigated materials only differed in their nitrogen content, it has been unequivocally demonstrated that the increased presence of nitrogen is responsible for the enhanced adsorption of CO2. The low-temperature nitrogen plasma treatment of activated carbon is a promising method for enhancing CO2 capture.