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Population growth and urbanization over the coming decades are anticipated to drive unprecedented demand for infrastructure materials and energy resources. Unfortunately, factors such as the degree of resource consumption, the energy-intensive nature of production, and the chemical-reaction driven emissions make infrastructure materials production industries among the greatest contributors to anthropogenic CO2 emissions. Yet there is an often-overlooked potential environmental benefit to infrastructure materials: most remain in use for decades and their long service lives can facilitate extended storage of carbon. In this perspective, we present an overview of recent technological advancements that can support infrastructure materials acting as a global, distributed carbon sink and discuss areas for further research and development. We present mechanisms to quantify the extent to which the embodied carbon will be removed from the carbon cycle for a long enough period of time to provide carbon sequestration and climate benefit. We conclude that it is possible to unlock the vast potential to engineer a carbon sequestration system that simultaneously meets societal need for expanding infrastructure systems; however, complexities in how these systems are engineered must be systematically and quantitatively incorporated into materials design.