The behavior of mixed samples (activated sludge and wastewater) was investigated after the addition of magnetite nanoparticles (NP-magnetite) in jar-tests, with objective to increase the aggregation of sludge and improve its settleability, aiming future application in granular sequencing batch reactors (SBR). The NP-magnetite was synthesized by the method of ion co-precipitation of Fe2+ and Fe3+ and characterized. The process of sludge sedimentation was evaluated for two different experimental strategies, with NP-magnetite concentrations between 25 and 150 mg L−1. The concentration of 75 mg L−1 was the most favorable to process, as evidenced by sludge volumetric index (SVI) and density. The results presented indicate that the addition of nanoparticles has the potential to improve aerobic granular systems increasing the settleability of seed sludge.