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This paper presents an experimental investigation on the mechanical properties and microstructure of geopolymer repair materials mixed using fly ash (FA) and concrete substrates. An optimal combination of FA and concrete substrate was determined using the compressive test of geopolymer mortar mixed with various concrete substrate classes. It was found that the contribution of (C35/45) concrete substrates with the FA geopolymer mortar increases the 28-day bonding strength by 25.74 MPa. The microstructure analysis of the samples using scanning electron microscopy showed the denser structure owing to the availability of high calcium and iron elements distribution. These metal cations (Ca2+ and Fe3+) are available at OPC concrete substrate as a result from the hydration process reacted with alumina-silica sources of FA and formed calcium aluminate silicate hydrate (C-A-S-H) gels and Fe-bonding linkages.