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Geopolymer binders have good potential in the repair of existing concrete structures due to their superior durability and mechanical performances. Understanding the interfacial transition zone (ITZ) between geopolymer mortars and ordinary Portland cement concrete is a crucial step to implement such an environmentally-friendly technology. This paper focuses on the failure modes of the bond interface and the microscopic and chemical interactions between various geopolymer mortars and concrete substrates at ITZs. The occurrence of newly-formed gels and second hydration mechanisms at ITZs are analyzed and discussed.