This report describes the application of various nuclear magnetic resonance (NMR) techniques to study the hydration kinetics and mechanisms, the structural properties, and the adsorption characteristics of coal fly ash. Coal fly ash samples were obtained from the Dave Johnston and Laramie River electric power generating plants in Wyoming. Hydrogen NMR relaxation times were measured as a function of time to observe the kinetics of hydration for the two coal fly ashes at different temperatures and water-to-cement ration. The kinetic data for the hydrated coal fly ashes were compared to the hydration of portland cement. The mechanism used to describe the kinetic data for the hydration of portland cement was applied, with reservation, to describe the hydration of the coal fly ashes. The results showed that the coal fly ashes differ kinetically from that of portland cement and from each other. Consequently, both coal fly ashes were judged to be poorer cementitious materials than portland cement. Carbon-13 NMR CP/MAS spectra were obtained for the anhydrous coal fly ashes in an effort to determine the type of organic species that may be present, either adsorbed on the surface or entrained.