This contribution describes the effect of the quality of the catalyst coating of cathodes for wastewater treatment by microbial fuel cells (MFC). The increase in coating quality led to a strong increase in MFC performance in terms of peak power density and long-term stability. This more uniform coating was realized by an airbrush coating method for applying a self-developed polymeric solution containing different catalysts (MnO2, MoS2, Co3O4). In addition to the possible automation of the presented coating, this method did not require a calcination step. A cathode coated with catalysts, for instance, MnO2/MoS2 (weight ratio 2:1), by airbrush method reached a peak and long-term power density of 320 and 200−240 mW/m2, respectively, in a two-chamber MFC. The long-term performance was approximately three times higher than a cathode with the same catalyst system but coated with the former paintbrush method on a smaller cathode surface area. This extraordinary increase in MFC performance confirmed the high impact of catalyst coating quality, which could be stronger than variations in catalyst concentration and composition, as well as in cathode surface area.