Solid oxide fuel cells that operate at intermediate temperatures require efficient catalysts to enhance the inherently poor electrochemical activity of the composite electrodes. Here, we present a simple and practical electrochemical deposition method for fabricating a PrOx overlayer on lanthanum strontium manganite–yttria‐stabilized zirconia (LSM–YSZ) composite electrodes. The method requires less than four minutes for completion and can be carried out under at ambient temperature and pressure. Crucially, the treatment significantly improves the electrode's performance without requiring heat treatment or other supplementary processes. The PrOx‐coated LSM–YSZ electrode exhibits an 89% decrease in the polarization resistance at 650 °C (compared to an untreated electrode), maintaining a 10‐fold reduction after approximately 400 h. Transmission line model analysis using impedance spectra confirms how PrOx coating improved the oxygen reduction reaction activity. Further, tests with anode‐supported single cells reveal an outstanding peak power density compared to those of other LSM–YSZ‐based cathodes (e.g., 418 mW cm−2 at 650 °C). Furthermore, we demonstrate that multicomponent coating, such as (Pr,Ce)Ox, can also be obtained with this method. Overall, our observations offer a promising route for the development of high‐performance solid oxide fuel cells.This article is protected by copyright. All rights reserved