Our experimentally validated MD simulations of gas permeability confirm the ML predictions, which suggests that many of the polymer candidates discovered here can be translated to reality in experiments. As elaborated upon in Fig. of Supporting Information, each of the promising polyimides identified here have a well-defined cross-linking formation from existing PubChem chemicals, which makes their syntheses tractable. However, the difficulty of synthesizing complex polymers in a solution-processable manner should not be underestimated. Therefore, to facilitate the overcoming of this challenge, we have tabulated the thousands of promising polymers that we have identified and included them in the GitHub repository associated with this work (), which we encourage experimental and computational researchers to explore further. While our models consider membrane performance to be constant, future efforts should also take into account how aging, plasticization, and swelling can degrade membrane performance over time, which is an important consideration in membrane design .