The electrochemical reversibility of the inserted redox probe plays a crucial role in the stability of the system. Our study reveals that Fc12-Br/MO lost electrochemical reversibility over continuous redox cycles, which hinders its potential as a biosensing platform. Through, in-situ SANS experiments, we identified the localization of Fc12-Br molecules within the MO cubic phase during potential-hold and continuous electrochemical cycling. Although no leaching of Fc12-Br or localized phase transitions were observed, the Br -counterions induced the formation of layer at the electrode surface that we propose is linked to the decay in electrochemical signals.