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Carbon capture in a postcombustion scenario needs cost-effective and energy-efficient alternatives to the amine process. High performance membranes can potentially meet the stringent cost targets set by the U.S. Department of Energy (DOE). In this context, we review and identify the most promising membranes/membrane materials along with the most innovative membrane-based processes reported recently in literature. The important transport results were grouped into different categories depending upon the mechanism of selective CO2 transport through the respective membrane. The analysis of the literature results indicates that each type of membrane demonstrates one or more of the important trade-offs including selectivity–permeability, selectivity–permeance, transport-ease of synthesis, and transport–stability. Reproducible and large-scale production of thin films from existing and new highly permeable materials while maintaining a reasonable selectivity along with innovation in process schemes that utilize multiple membranes with different and unique benefits were identified as key tasks to realizing a membrane-based alternative for this application.