For several decades, class F fly ash has been an attractive supplementary cementitious material, at least in part, due to its ability to reduce Portland cement consumption and mitigate alkali-silica reactions in concrete. However, fly ash availability is becoming uncertain as the energy industry decommissions coal burning power plants as it transitions to renewable energy production. This situation creates a need to identify viable and sustainable alternative supplementary cementitious materials. There are several types of supplementary cementitious materials, such as natural pozzolans, metakaolin, or ground granulated blast-furnace slag, which appear to be potential alternatives to fly ash in concrete. In this research, a locally available natural pozzolan (pumicite) was selected to replace fly ash in concrete. After conducting alkali-silica reaction tests on mortar mixtures, rheological and strength properties, shrinkage, resistance to freezing and thawing, and chloride ion permeability of concrete mixtures containing different amounts of fly ash and natural pozzolan were evaluated. The results showed that pumicite was more effective than fly ash at mitigating the alkali-silica reaction, and a pumicite content of 20% was necessary to mitigate the alkali-silica reaction. Ternary mixtures containing both pumicite and fly ash were the most effective cementitious materials combinations for mitigating the alkali-silica reaction expansion. Additionally, pumicite provided acceptable compressive strength and modulus of rupture values (greater than 4.0 MPa) that exceeded the flexural strengths provided by established mixtures containing only fly ash. Shrinkage and durability factor values for all mixtures were less than 710 μstrain and greater than 75, which are generally considered acceptable. Additionally, all mixtures with acceptable alkali-silica reaction expansions had very low chloride permeability. These results indicate that pumicite can be a reliable alternative for fly ash.