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Products from chemical engineering are essential for human well-being, but they also contribute to the degradation of ecosystem goods and services that are essential for sustaining all human activities. To contribute to sustainability, chemical engineering needs to address this paradox by developing chemical products and processes that meet the needs of present and future generations. Unintended harm of chemical engineering has usually appeared outside the discipline's traditional system boundary due to shifting of impacts across space, time, flows, or disciplines, and exceeding nature's capacity to supply goods and services. Being a subdiscipline of chemical engineering, process systems engineering (PSE) is best suited for ensuring that chemical engineering makes net positive contributions to sustainable development. This article reviews the role of PSE in the quest toward a sustainable chemical engineering. It focuses on advances in metrics, process design, product design, and process dynamics and control toward sustainability. Efforts toward contributing to this quest have already expanded the boundary of PSE to consider economic, environmental, and societal aspects of processes, products, and their life cycles. Future efforts need to account for the role of ecosystems in supporting industrial activities, and the effects of human behavior and markets on the environmental impacts of chemical products. Close interaction is needed between the reductionism of chemical engineering science and the holism of process systems engineering, along with a shift in the engineering paradigm from wanting to dominate nature to learning from it and respecting its limits.