Canada produces about one-third of the global supply of medical radioisotopes. The nuclear power reactors in Ontario, Quebec and New Brunswick have generated about 17 percent of the electricity in the country every year (NWMO, 2010; Noorden; 2013). Since the 1960s, more than 2 million used (or spent) fuel bundles (high-level radioactivity) and 75,000 m³ of low- and intermediate-level radioactive waste have been produced, which is increasing by 2000 to 3000 m³ every year after reducing the processed volume (Jensen et al., 2009). More than 30 countries around the world, including Canada, have proposed construction of very deep geological repositories (DGRs) to store this nuclear waste for design periods 1,000,000 years. DGR concepts under development in Canada (the DGR is likely to be constructed in Ontario) are based on a multi-barrier system (NWMO, 2012). A crucial component of the multi-barrier system is the engineered barrier system (EBS), which includes a buffer, backfill, and tunnel sealing materials to physically, chemically, hydraulically and biologically isolate the nuclear waste. Bentonite-based material has been chosen for this critical use because of its high swelling capacity, low hydraulic conductivity, and for its good ability to retain radionuclides in the case of failed canisters. However, the presence of bentonite-based material in DGRs, surrounded by an aggressive environment of underground saline water, nuclear waste heat decay, and corrosion products under confining stress, may lead to mineralogical changes. Consequently, the physical and physiochemical properties of bentonite-based materials may change, which could influence the performance of bentonite in an EBS as well as the overall safety of DGRs. The objective of this research is to investigate the impact of the underground water salinity, heat generated by nuclear waste, and corrosion products of nuclear waste containers in Ontario on the engineering and micro-/nano-structural properties of bentonite-sand engineered barrier materials. Free-swelling, swelling pressure and hydraulic conductivity tests have been performed on bentonite-sand mixtures subjected to various chemical (groundwater chemistry; corrosion water with iron as a corrosion product) and thermal (heat generated) conditions. Several techniques of micro- and nano-structural analyses, such as x-ray diffraction (XRD), X-Ray microanalysis (DES), surface area and pore size distribution analyses (BET, BJH) and differential gravimetric (TGA and DTG) analyses have also been conducted on the bentonite-sand materials. Valuable results have been obtained for better understanding the durability and performance of the bentonite-sand barrier for the DGR which may be located in Ontario. The obtained results have shown that the groundwater chemistry and corrosion products of the nuclear containers significantly deteriorate the swelling and permeability properties of the tested bentonite-sand barrier materials, while temperature has little or no effect.