The activated sludge process is the most widespread sewage treatment method. It typically consists of a pretreatment step, followed by a primary settling tank, an aerobic degradation process, and, finally, a secondary settling tank. The secondary effluent is then usually chlorinated and discharged to a water body. Tertiary treatment aims at improving the characteristics of the secondary effluent to facilitate its reuse. In this work, through a literature review of the most prominent tertiary treatment methods, a benchmarking of their technical efficiency, economic feasibility, and environmental impact was carried out. The photo-Fenton method proved to be the most technically efficient process, significantly reducing the microbial load and pharmaceutical content (by 4.9 log and 84%, respectively) of the secondary effluent. Chlorination and UV irradiation exhibited the lowest treatment costs (0.004 EUR/m−3) and the lowest global warming potential (0.04 and 0.09 kg CO2eq. m−3, respectively). After all the data were aggregated, a decision-making tool was constructed in the form of a ternary diagram, which indicates the most appropriate tertiary treatment method according to the weight-per-process aspect (technical, economic, and environmental) selected by the user, with chlorination, UV irradiation, ozonation, microalgae cultivation, and constructed wetlands prevailing in the final results.