Municipal wastewater treatment plants (MWWTPs) are essential infrastructures in any urban context, but they may be considered as a potential source of greenhouse gas (GHG) emissions and should be coherent with European Union (EU) policy on energy efficiency. This study presents a sustainability evaluation of four Italian and Romanian MWWTPs in terms of energy efficiency and greenhouse gas emissions using Energy Performance and Carbon Emissions Assessment and Monitoring (ECAM) tool software. The obtained results indicated that biogas recovery improved energy performances, while the largest contributions in terms of GHG emissions were in all cases caused by energy consumption and methane produced during wastewater treatment. The Romanian plants exhibited higher GHG emissions, compared to the Italian plants, mainly because of the different values of national conversion factors for grid electricity (0.41 kg CO2/kWh for Italy and 1.07 kg CO2/kWh for Romania). Two scenarios aimed at enhancing the overall sustainability were hypothesized, based on increasing the serviced population or energy efficiency, achieving significant improvements. A sustainability assessment of MWWTPs should be adopted as a useful tool to help water utilities to introduce low-energy, low-carbon management practices as well as being useful for policy recommendations.