This study examined the applicability of two mine sludge wastes, mine tailing sludge (MTS) and acid mine drainage sludge (AMDS) as iron-rich bio-stimulant for enhancing organic matter degradation in anaerobic process. Batch treatment of domestic sewage having 343 ± 10 mg/L chemical oxygen demand (COD) using MTS and AMDS as additives mixed with septic tank sludge as anaerobic inoculum produced lower start-up time, higher efficiency of COD removal, enhanced biomass retention, and higher acidogenic and methanogenic activity after stabilization. Biostimulation induced by mine sludge waste additives in anaerobic system were observed to have correlation with percentage of iron content in the additives, as well as difference in surface charge between biomass and the additives. Treatment efficiency induced by the two mine sludge waste based additives were similar at 90% confidence limit, however, was found to be higher than lower iron containing additive laterite soil, while lower than higher iron containing synthetic zero valent nano iron as additives used for comparison. The study was supported by scanning electron microscope, atomic force microscope and optical microscope images of sludge granule sand surface charge measurement.