This study aimed to verify if coal ash, a residue from thermal power plants, could act as a granulation nucleus, cations source, and abrasive element to favor granules formation and stability in aerobic granular sludge (AGS) systems. Two simultaneous fill/draw sequencing batch reactors (SBRs) (R1 and R2) were operated with 6-h cycles, i.e., the filling and drawing phases occurred simultaneously, followed by the reaction and settling phases. R1 was maintained as control, while R2 was supplemented with coal ash (1 g·L-1) on the first day of operation. Granulation was achieved in both reactors, and no significant differences were observed in terms of settleability, biomass retention, morphology, resistance to shear, and composition of the EPS matrix. However, the ash addition did not change the settleability, biomass retention, granule morphology, shear resistance, and extracellular polymeric substances (EPS) content significantly. COD removal was high (≥ 90%), while nitrogen (~50%) and phosphorus (~40%) removals were low, possibly due to the presence of nitrate during the anaerobic phase. With granulation, microbial population profile was altered, mainly at the genus level. In general, the operational conditions had a more considerable influence over granulation than the ash addition. The possible reasons are because the ash supplementation was performed in a single step, the low sedimentation rate of this particular residue, and the weak interaction between the ash and the EPS formed in the granular sludge. These factors appear to have decreased or prevented the action of the ash as granulation nucleus, source of cations, and abrasive element.