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Globally, the production of concrete is responsible for 5% to 8% of anthropogenic CO2 emissions. Cement, a primary ingredient in concrete, forms a glue that holds concrete together when combined with water. Cement embodies approximately 90% of the greenhouse gas emissions associated with concrete production, and decarbonization methods focus primarily on cement production. But mitigation strategies can accrue throughout the concrete life cycle. Decarbonization strategies in cement manufacture, use, and disposal can be rapidly implemented to address the global challenge of equitably meeting societal needs and climate goals. This review describes (a) the development of our reliance on cement and concrete and the consequent environmental impacts, (b) pathways to decarbonization throughout the concrete value chain, and (c) alternative resources that can be leveraged to further reduce emissions while meeting global demands. We close by highlighting a research agenda to mitigate the climate damages from our continued dependence on cement.