This study investigated the potential of enhancing the activity of iron-reducing bacteria (IRBs) to increase the biomethanation rate of waste activate sludge (WAS). The effects of biostimulation by ferric oxyhydroxide (Phase 2) and bioaugmentation with an enriched IRB consortium (Phase 3) were examined in a continuous anaerobic reactor treating WAS. Compared to the control operation (Phase 1), significant rises in methane yield (10.8-59.4%) and production rate (24.5-52.9%) were demonstrated by the biostimulation and bioaugmentation treatments. Visible structural changes were observed in bacterial community with the phases while not in archaeal community. Acinetobacter-and Spirochaetales-related populations were likely the major players driving anaerobic iron respiration and thus leading to enhanced biomethanation performance, in Phases 2 and 3, respectively. Our results suggest an interesting new potential for enhancing biomethanation of WAS. (C) 2014 Elsevier Ltd. All rights reserved.