Three activated sludge reactors were operated to improve the removal of organic micropollutants such as Pharmaceutical and Personal Care Products (PPCPs). Reactor 1 (R1) was operated as a Conventional Activated Sludge reactor (CAS), Reactor 2 (R2) consisted of a CAS unit that was continuously fed with FeCl3 whereas granular activated carbon (GAC) was fed directly into the mixed liquor of Reactor 3 (R3) in order to attain concentrations in the range 100-1,000 mg/L. PPCPs removal rates varied depending on the compound present in each reactor during the entire 220 days of operation. Some substances showed the same behaviour in all reactors, such as the acidic pharmaceuticals naproxen and ibuprofen, which were almost completely removed (> 90%). More hydrophobic organic substances, like musk fragrances, were about 90% removed after 40 days of operation in all of the reactors. The main difference between the three reactors was obtained in R3 when the GAC concentrations in the aeration tank were around 500-1,000 mg/L. Under these conditions, the more recalcitrant compounds like diazepam and carbamazepine could be removed by up to 40%, and diclofenac up to 85%. Adsorption isotherms for PPCPs were obtained with activated carbon, and the results were successfully fitted to the Freundlinch equation. The more recalcitrant compounds (carbamazepine, diazepam and diclofenac) had the highest adsorption capacities onto GAC, which is consistent with the behaviour observed in R3 and helps to identify the removal mechanism (adsorption for these compounds, whereas absorption for fragrances).