The adverse effect of illite clay on bitumen recovery was found to be related to its acidity. The addition of calcium or magnesium ions to the flotation deionized water had a marginal effect on bitumen recovery when measured using a Denver flotation cell. However, the co-addition of illite clay and divalent cations caused a significant reduction in bitumen recovery. The effect was found to be compounded at a lower process temperature and low pH values. Zeta potential distributions of illite suspensions and bitumen emulsions were measured individually and as a mixture to investigate the effect of divalent cations on the interaction between bitumen and illite clay. The presence of I mM calcium or magnesium ions in deionized water had a significant effect on the interactions between bitumen and illite clay. Slime coating of illite onto bitumen was not observed in zeta potential distribution measurements performed in alkaline tailings water.