In the present study, a hybrid Al(OH)(3)-polyacrylamide (Al-PAM) was synthesized and used in combination with a partially hydrolyzed polyacrylamide (HPAM) to process a low-grade oil sand ore. It was found that Al-PAM was capable to improve bitumen froth quality and tailings settling. But it led to deterioration in bitumen recovery due to the formation of large bitumen lumps during the bitumen extraction process. To resolve this problem, HPAM was added in combination with Al-PAM as a dual system. The use of the dual system at a low dosage achieved a holistic improvement in bitumen recovery, froth quality, and tailings settling. To understand the role of Al-PAM and the dual system in the bitumen extraction process, bitumen-clay, bitumen-bitumen, and clay-sand interaction and adhesion forces were directly measured using an atomic force microscope (AFM). The measured forces indicate that bitumen recovery and tailings settling are controlled by the colloidal interaction and adhesion forces between the oil sand components.