Two 1,2,3-triazolium ionic liquid diluents were evaluated for the extraction of gallium from spent Bayer process liquor by Kelex® 100. The first of these is a hydrophobic ionic liquid with a low water content, which allows the extraction of gallium directly from untreated Bayer process liquor. The second is based on a hydrophilic ionic liquid and which forms an aqueous biphasic system with concentrated salt solutions. The aqueous biphasic system homogenizes upon cooling, which allows homogeneous liquid-liquid extraction of gallium from carbonated Bayer process liquors. The influence of the ionic liquids on the extraction kinetics, mechanism, thermodynamics and selectivity is investigated. Stripping was examined from both systems and their potential for industrialization is discussed. Ionic liquids are shown to beneficially influence the extraction process from thermodynamic and kinetic perspectives. They are therefore promising to solve the issues which have thus far prevented the industrial application of resource-efficient solvent extraction techniques for the recovery of gallium from spent Bayer process liquor.