This study introduces an innovative approach to designing membranes capable of separating CO2 from industrial gas streams at higher temperatures. The novel membrane design seeks to leverage the well-researched high-temperature CO2 adsorbent, hydrotalcite, by transforming it into a membrane. This is achieved by combining it with an amorphous organo-silica-based matrix, extending the polymer-based Mixed Matrix Membrane concept to inorganic compounds. Following the membrane material preparation and investigation of the individual membrane in Part 1 of this study, we examine its permeation and selectivity here. The pure 200 nm thick hydrotalcite membrane exhibits Knudsen behavior due to large intercrystalline pores. In contrast, the organo-silica membrane demonstrates a permselectivity of 13.5 and permeance for CO2 of 1.3 107 mol m2 s1 Pa1 at 25°C, at 150°C the good separation behavior is reduced. Combining both components results in a hybrid microstructure, featuring selective surface diffusion in the microporous regions and unselective Knudsen diffusion in the mesoporous regions. Further attempts to bridge both components to form a purely microporous microstructure are outlined.