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Polymer membranes employed in gas separation play a pivotal role in advancing environmental sustainability, energy production, and gas purification technologies. Despite their significance, the current design and manufacturing of these membranes lack cradle-to-cradle approaches, contributing to plastic waste pollution. This study explores emerging solutions, including the use of biodegradable biopolymers such as polyhydroxybutyrate (PHB) and membrane recycling, with a focus on the specific impact of mechanical recycling on the performance of biodegradable gas separation membranes. This research represents the first systematic exploration of recycling biodegradable membranes for gas separation. Demonstrating that PHB membranes can be recycled and remanufactured without solvents using hot-melt extrusion and 3D printing, the research highlights PHB's promising performance in developing more sustainable CO 2 separations, despite an increase in gas permeability with successive recycling steps due to reduced polymer molecular weight. The study emphasizes the excellent thermal, chemical, and mechanical stability of PHB membranes, albeit with a marginal reduction in gas selectivity upon recycling. However, limitations in PHB's molecular weight affecting extrudability and processability restrict the recycling to three cycles. Anticipating that this study will serve as a foundational exploration, we foresee more sophisticated recycling studies for gas separation membranes, paving the way for a circular economy in future membrane technologies., Competing Interests: The authors declare no competing financial interest., (© 2024 The Authors. Published by American Chemical Society.)