This work focuses on developing a new adsorptive material and regenerable system for CO2 sequestration to supply CO2-free gas stream for low temperature and low carbon dioxide concentration applications, such as alkaline fuel cells, metal-air batteries, and portable air-purifying respirators. A novel microfibrous media has been introduced for carbon dioxide filtration from wet gas streams at room temperature. The use of microfibrous media in a composite bed maximizes the breakthrough capacity per unit volume and promotes high accessibility. The microfibrous media synergically combines the high contacting efficiency of the microfibrous matrix and the small internal mass transfer resistance of small particulates. The carbon dioxide adsorption capacity of the microfibrous media can be reversibly recovered. The incorporation of microfibrous media to the sodalime was observed. The result shows 120% improvement in the breakthrough capacity compared with the packed bed of the sodalime with the same volume. This approach can be applied to miniaturize the reactor and reduce thermal mass enhancing process intensification.