Concrete is integral to building and maintaining transportation infrastructure, but it is also responsible for nearly 10% of human-caused greenhouse gas (GHG) emissions. Most of these emissions are from cement production (70-90%). As 30% of cement consumption is for transportation infrastructure, the impacts of concrete need to be reduced to develop enable sustainable transportation systems. Typically, replace cement with supplementary cementitious materials (SCMs) (e.g., fly ash from coal combustion or slag from pig iron production) is used to reduce GHG emissions. However, the supply of conventional SCMs is restricted. Society needs additional SCM resources to meet the demand for concrete materials while also complying with legislative requirements to reach net-zero cement GHG emissions by 2045. This work concurrently evaluates unconventional SCMs using industrial ecology techniques (i.e., life cycle assessment and material flow analysis) and experimentally determined mechanical performance metrics. This dissertation will present an evaluation framework, using material from California as a case study, to prioritize the adoption of SCM by concurrently considering (1) material performance, (2) resource availability, and (3) environmental impact reduction. Environmental impacts and global warming disproportionally affect historically marginalized and low-income communities. Thus, by enabling more sustainable concretes, this dissertation aligns with NCST and PSR UTC goals to develop more equitable and more sustainable transportation systems.