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Fly ash (FA) and Basic oxygen furnace (BOF) slag were used to as additives in the geopolymerisation of gold mine tailings (GMT).The aim of the research was to determine the effects of the two additives on the strength formation and mechanism of metal immobilisation by modified GMT geopolymers. GMT, FA and BOF were mixed, respectively, and made into a paste with the addition of potassium hydroxide (KOH) before curing at various conditions. 50% replacement of GMT in the starting materials gave the highest unconfined compressive strength (UCS). The UCS for BOF-based geopolymer was 21.44 Mega Pascals (MPa), whilst the one for FA-based geopolymer was 12.98 MPa. The BOF-based geopolymer cured at lower temperature (70 °C) as compared to the FA-based geopolymer (90 °C). The optimum KOH concentration was 10 and 15 M for BOF-and FA-based geopolymers, respectively. BOF-based geopolymers resulted in the formation of calcium silicate hydrate (CSH) phases which contributed to higher strength; whereas in FA-based geopolymers, no new structures were formed. BOF-based geopolymers resulted in over 94% iron (Fe) immobilisation, whereas FA-based geopolymers had 76% Fe immobilisation. Fe immobilisation was via incorporation into the CSH or geopolymer structure, whilst other metal immobilisations were thought to be via encapsulation. 12-month static leaching tests showed that the synthesised geopolymers posed insignificant environmental pollution threat for long-term use.