The manufacturing, operation, and disposal of computing systems are increasingly impacting the environment. Traditionally, computing systems are designed to maximize energy efficiency and job performance, while elements such as greenhouse gas emissions and electronic waste continue to trend upward. These factors are dependent on the underlying dynamics of the computing systems, and time-sensitive reactions have the potential to address these issues. This project tackles the sustainability of computing systems using dynamic system optimization, setting an explicit focus on critical sustainability metrics for designing future computing systems. An emphasis is placed on pushing forward the scientific understanding of sustainable computing systems, and to impact future critical structures such as datacenters. This project serves to support not only the computing field, but also provides advancements in the design and controls fields. The outcomes of the project also support education of scientific communities and the public alike through expansive multimedia resource development and student training.<br/><br/>Three aims are defined for this research. The first aim is to improve and reformulate models of sustainable computing systems for integration within optimization, addressed by development of a methodology to convert data-driven surrogate models into dynamic analysis-friendly formats. The second aim is to understand and quantify the impact different representations of sustainability metrics have on optimization problem solution feasibility. This is pursued through categorization of sustainability metrics for automatic generation of solvable optimization problems. The third aim is to develop and evaluate the capabilities of dynamic system optimization for sustainability-centric computing systems, using a novel framework. Validation is performed through a combination of numerical and experimental case studies, ranging from server cooling to datacenter design. The potential contributions of studying computing systems through dynamic system optimization are large, discrete jumps in sustainability metrics, such as reductions in emissions, waste heat, and electronic waste.<br/><br/>This award reflects NSF's statutory mission and has been deemed worthy of support through evaluation using the Foundation's intellectual merit and broader impacts review criteria.