Composite polymer membranes were prepared using carbonate, polyvinyl alcohol, an acrylic acid polymer partial sodium salt cross-linked product, and sodium polyacrylate.In this study, the factors for further improving the separation performance of these membranes for the CO 2 /He mixed gas were investigated. It was confirmed that the prepared membranes did not provide stable separation under pressure unless they had a thickness of 2.0 μm. Moreover, they could not function as high-performance separation membranes without a carbonate additive; the optimal carbonate concentration range was determined by considering the effect of the total pressure. As a result, this work produced a high-performance, CO 2 selective permeable membrane with selectivities of more than 500 and 150 at 0.1 and 0.7 MPa, respectively, for the separation of a CO 2 /He (80/20) gas mixture at 85 C.