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Thin-film composite (TFC) membranes containing various fillers and additives present an effective alternative to conventional dense polymer membranes, which often suffer from low permeance (flux) and the permeability–selectivity tradeoff. Alongside the development and utilization of numerous new polymers over the past few decades, diverse additives such as metal–organic frameworks (MOFs), graphene oxides (GOs), and ionic liquids (ILs) have been integrated into the polymer matrix to enhance performance. However, achieving desirable interfacial compatibility between these additives and the host polymer matrix, particularly in TFC structures, remains a significant challenge. This review discusses recent advancements in TFC membranes for CO2/N2 separation, focusing on material structure, polymer–additive interaction, interface and separation properties. Specifically, we examine membranes operating under dry conditions to clearly assess the impact of additives on membrane properties and performance. Additionally, we provide a perspective on future research directions for designing high-performance membrane materials. [ABSTRACT FROM AUTHOR]