OverviewThe discovery, development, and deployment of sustainable polymers, the molecules that make up plastics, are critical to the health of the globe and its inhabitants. Moreover, the economic vitality of the multitudinous industries that use polymers in their processes and products will be critically reliant on sustainable solutions because of many interwoven factors that include environmental stewardship, policy compliance, and societal and investor demands. Stakeholders in the polymeric materials ecosystem clearly recognize the significant motivating factors in a push to meet the requirements of a circular economy and thus a sustainable future. Inertia associated with the current polymer production and consumption landscapes, however, has resulted in resistance toward change that has proven challenging to overcome. Factors that have contributed to the status quo include the ubiquitous nature of plastics utilization across all sectors of the economy, the incredibly diverse and tunable functional attributes of polymeric materials that make them desirable to other material alternatives, and the highly optimized and economic mass manufacturing capabilities associated with plastics derived from low-cost petroleum resources. There is an urgent need for change to solve our pressing plastics predicament: modern society depends on these polymeric materials and continually expects increased performance and functionality but suffers dire consequences from the associated pollution, which takes the forms that include greenhouse gas emissions from plastic production, and accumulation of plastic waste in the environment. A solution to this polymer puzzle is imperative.Given the current advantages of plastics in modern society and the clear recognition of the everaccumulating waste associated with their disposal, lack of efficient recycling technologies and infrastructure, and persistence in the environment, it is clear that a new approach is needed We are motivated by the successes associated with the Materials Genome Initiative (MGI), 1 where the close coupling of experiment and theory has facilitated materials discovery in some sectors. But while an MGI approach has been effective at accelerating the research cycle of prediction, synthesis, and characterization, efforts to incorporate the elements of translation and technological deployment into that cycle have been limited. This is especially true in the soft materials arena. If a next-generation MGI-like approach spanning length scales (from atomic to molecular to material) and time scales (from nanoseconds to decades) can be envisioned, implemented, and supported, and if attention is given to technological feasibility, it will serve as