The present study investigates the effects and mechanisms of aluminum (Al(III)) and iron (Fe(III)) ions on the flotation efficiency of potassium feldspar (K-feldspar) within oleate collector systems. The study employs micro-flotation experiments, solution chemistry calculations, zeta potential measurements, and FT-IR and XPS analyses to demonstrate that Al(III) and Fe(III) ions can significantly improve the flotation recovery of K-feldspar by altering its surface charge, bonding properties, and adsorption modes. The study also develops adsorption models for the flotation of K-feldspar activated by Al(III) and Fe(III), revealing the synergistic impacts of metal ion hydrolysis products and sodium oleate in the formation of hydrophobic complexes.