The efficiency by which monomers may be recovered during the chemical recycling of plastic waste has thus far dominated the discussion over which future polymer chemistries might be more sustainable than those in use today. However, at scale, other factors emerge as equally important, such as the costs of primary versus secondary resin production as well as the energy and carbon intensity of circular manufacturing processes. We apply systems analysis to identify problematic chemical processes used for the primary production of plastics designed for infinite recyclability: polydiketoenamine (PDK) resins from novel triketone and amine monomers. Leveraging this knowledge, we advance a less intensive process for triketone production, which lowers the cost of primary PDK production by 57% and results in 66% less life-cycle greenhouse gas (GHG) emissions. Using the automotive sector as a case study, we discuss the impact of replacing nonrecyclable polyurethane with circular PDK over the next 60 years. We find that the cumulative GHG emissions associated with introducing PDK are half those of staying the course with polyurethane. However, the extent to which circularity is realized through targeted collection and sorting plays the dominant role in determining how much of those savings is practically achievable.