A detailed laboratory study was conducted to investigate the properties of cement-fly ash grout mixtures as barriers for isolation of hazardous and low-level radioactive wastes. In the grout studied, fly ash was used to replace 30 percent by mass of cement. Three additives including bentonite, silica fume, and polypropylene fiber were used individually in the grout mixes to improve the properties of the grouts in different aspects. The flowability, bleeding, and setting time of freshly mixed grouts were determined; and the unconfined compressive strength, pore size distribution, and water permeability were determined for hardened grouts at various curing durations up to 120 days. Finally, the durability of cement-fly ash grouts was carefully examined in terms of the changes in their physical properties after different levels of exposure to sulfate attack and wet-dry cycles.