{Reference Type}: Journal Article {Title}: Toward a Circular Bioeconomy: Designing Microbes and Polymers for Biodegradation. {Author}: Mubayi V;Ahern CB;Calusinska M;O'Malley MA; {Journal}: ACS Synth Biol {Volume}: 0 {Issue}: 0 {Year}: 2024 Jun 25 {Factor}: 5.249 {DOI}: 10.1021/acssynbio.4c00077 {Abstract}: Polymer production is rapidly increasing, but there are no large-scale technologies available to effectively mitigate the massive accumulation of these recalcitrant materials. One potential solution is the development of a carbon-neutral polymer life cycle, where microorganisms convert plant biomass to chemicals, which are used to synthesize biodegradable materials that ultimately contribute to the growth of new plants. Realizing a circular carbon life cycle requires the integration of knowledge across microbiology, bioengineering, materials science, and organic chemistry, which itself has hindered large-scale industrial advances. This review addresses the biodegradation status of common synthetic polymers, identifying novel microbes and enzymes capable of metabolizing these recalcitrant materials and engineering approaches to enhance their biodegradation pathways. Design considerations for the next generation of biodegradable polymers are also reviewed, and finally, opportunities to apply findings from lignocellulosic biodegradation to the design and biodegradation of similarly recalcitrant synthetic polymers are discussed.