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Although aliphatic polycarbonates (APCs) have been proposed as alternative materials for films, packaging, and rigid plastics applications, their industrial applications are limited to low-molecular-weight polycarbonate polyols, macromonomers for the production of polyurethanes, and other copolymers. The selective transformation of epoxides and carbon dioxide, one of the most abundant and renewable carbon resources, into degradable polycarbonates is a promising green and sustainable route to polycarbonates. The review by Jianwen Xu, Ellva Feng, and Jie Song summarizes the latest polymerization techniques for preparing well-defined functional APCs and their new applications, especially in the biomedical field. The cover photo is taken from the macromer synthesis, crosslinking, and cell encapsulation strategies of a clickable APC-based hydrogel system developed by the authors. (DOI: 10.1002/app.39822)