“…This will not only fundamentally enable the next-generation bioelectrical sensing and actuation but also implore the need to characterize electrodes of various sizes and materials/coatings at subcellular levels. Considerable studies on modeling the electrode–electrolyte interfaces have established our understanding of the effects of various electrode properties, such as electrode materials and sizes, on the biosensing and electrical stimulation through MEAs. ,,,− Previous investigations have also demonstrated that non-uniform distribution of current near edges of electrodes often causes early electrode degradations. ,, Recently, conducting polymer-coated electrodes have been considered as an ideal alternative to conventional metal or metal-oxide electrodes. ,, Particularly, PEDOT:PSS-coated electrodes (>10 μm) have been shown to significantly reduce the interfacial impedance and thermal noise while maintaining long-term electrochemical stability and excellent biocompatibility due to its mixed electronic/ionic conductivity. ,,− ,,− In addition, the elastic nature of PEDOT:PSS reduces the mechanical mismatch at the interface between electrodes and cells, enhancing devices’ biocompatibility and decreasing their invasiveness . However, despite several decades of research, the performance limitations, electrochemical characteristics, and electrode–electrolyte interfaces attributed to electrodes of varying compositions, sizes, and polymer coatings have not been systematically characterized, especially for electrodes of subcellular sizes that exhibit substantial edge-to-area ratios.…”