Concerns over the future availability of traditional SCM sources, such as fly ash, have left the concrete industry in need of alternative sources of SCMs. The research presented here has evaluated natural pozzolans such as pumice, perlite, vitric ash, zeolites, shale and calcined clay as alternative sources of SCMs. Unlike previous research that has only concentrated on empirically evaluating the performance of natural pozzolans in concrete, the research presented in this dissertation has measured both the performance of the pozzolans in cementitious mixtures as well as their physical and chemical characteristics, to draw meaningful relationships between pozzolan properties and performance. The physical and chemical characteristics of these natural SCMs were measured using techniques like particle size analysis, Brunauer–Emmett–Teller (BET) surface area, scanning electron microscope (SEM) imaging, x-ray fluorescence (XRF), x-ray diffraction (XRD), and thermal gravimetric analysis (TGA). The performance of the pozzolans as alternative SCMs was examined by looking at their effect on mortar strength and mixture workability, as well as by their ability to mitigate expansions from durability problems like alkali silica reaction (ASR) and sulfate attack. The performance of the pozzolans was related back to their physical and chemical characteristics to gain an understanding of the underlying mechanisms of cement and pozzolan interaction, and to draw insights as to why some pozzolans perform better than others in cementitious mixtures. Using this knowledge, some of the under-performing pozzolans were modified to see if changes in their properties could improve performance. Results of the research showed that other than the two coarse zeolites, the rest of the pozzolans tested could be used as Class F fly ash replacements in concrete, with the pumice, perlite, metakaolin and fine zeolite being the best performers in terms of mortar strength and durability. Although the pumice mortar had lower strengths than the control at early ages, results from the performance improvement studies showed that the reactivity of pumice could be enhanced by grinding the pozzolans to a finer particle size distribution. Zeolites were found to negatively affect mixture workability, but calcination of the zeolites helped to improve the workability of zeolite mixtures. / text