The demand for portland cement concrete is expected to increase over time. There is a need to develop a more sustainable cementitious systems in order to reduce the negative environmental impacts associated with ordinary portland cement (OPC) production. An attempt is made to investigate sustainable binder solutions through the use of alternative cementitious materials at high levels of volume replacement. Limestone, an abundant material is used as a filler in low water-to-powder concretes where a substantial fraction of the portland cement remains unhydrated. At high volume OPC replacement, 20% and 35%, the combination of limestone and an alumina source has been shown to improve mechanical and durability performance. At 20% OPC replacement levels the migration coefficient which is an indication of chloride penetration in concrete is lower than the OPC control mixture at 28 and 56 days of hydration. The use of limestone with a similar particle size distribution to that of the OPC is used in each of these blended systems. A 20% binary limestone blend provide similar strength to an OPC mortar at all ages and comparable transport properties to that of the OPC concrete. Fly ash and metakaolin are the two alumina sources for the ternary blended mixes with concrete. The metakaolin shows the highest increase in the amount of hydration products formed out of all the mixes, including calcium-silicate-hydrate and carboaluminate phases in combination with limestone powder. At both levels of replacement the metakaolin blends show a substantially lower migration coefficient which is contributed to the smaller pore sizes found in the metakaolin blends. The fracture response of these systems show that at all replacement levels the ductility of the systems increase indicated by the large critical crack tip opening displacement. The fracture toughness is the highest for the blend containing metakaolin indicative of the smaller pore sizes allowing more dissipation of energy. An attempt is made to relate all mechanical and durability parameters to the reaction products and pore-structure developing at later ages.