Two inorganic-organic hybrid polymers, Al(OH)3-polyacrylamide (Al-PAM) and Fe(OH)3-polyacrylamide (Fe-PAM) were synthesized and used in flocculating model tailings (5 wt% kaolin suspensions) and laboratory extraction tailings. For comparison, a commercial anionic flocculant, partially hydrolyzed polyacrylamide or Magnafloc 1011 (MF 1011), was also examined. Moreover, a fundamental understanding on flocculation dynamics of model and laboratory extraction tailings by different polymers as well as adsorption kinetics of these polymers on different surfaces was established using focused beam reflectance measurement (FBRM) and quartz crystal microbalance with dissipation (QCM-D), respectively. For model tailings, Al-PAM, Fe-PAM and MF 1011 exhibited excellent flocculation efficiency, but MF 1011 was found to be sensitive to overdosing. For laboratory extraction tailings, hybrid polymers showed better flocculation performance than MF 1011. Adsorption measurement of polymers by QCM-D indicated that Fe-PAM adsorbed more significantly on bitumen than Al-PAM. Thus, with the presence of bitumen, Fe-PAM could be a better flocculant than Al-PAM in the treatment of oil sands tailings.