Molecular Design for Dual Circularity: Polyester with Complementary Mechanical and Chemical Recyclability under Mild Conditions

The plastic waste accumulation requires facile yet effective solutions. Currently mechanical recycling typically leads to downcycling, while the environmental footprint of chemical recycling is often unacceptable. Here, we introduce a dual circularity concept, where rational molecular design paves the way for complementary closed‐loop mechanical and chemical recyclability under mild conditions. Very small changes in macromolecular structures, thermal and mechanical properties were observed, after as many as six repeated mechanical recycling cycles, showing that a wide processing window could be the key for closing the mechanical recycling loop. Facile, time and energy efficient closed‐loop chemical recycling into products with identical performance to original ones was also realized, thanks to the abundant free volume and accessible ester‐functionalities. With these design criteria at hand, dual circulation in recyclability can be realized; proceeding with mechanical recycling when we can, and switching to chemical recycling when we must.