Embodiments of the present disclosure pertain to ion-selective electrodes that include a metal-organic framework and an electrode surface. The metal-organic framework is associated with the electrode surface in a manner that forms an interface between the metal-organic framework and the electrode surface. Additional embodiments pertain to methods of detecting an ion in a sample by associating the sample with the ion-selective electrodes of the present disclosure. The metal-organic frameworks of the ion-selective electrodes mediate ion-to-electron transduction through the interface between the metal-organic and the electrode surface. Thereafter, the presence or absence of the ion in the sample is detected by detecting a change in potential of the ion-selective electrode and correlating the change in the potential to the presence or absence of the ion. The metal organic frameworks may simultaneously mediate ion sensing and ion-to-electron transduction through the interface between the metal-organic frameworks and the electrode surface.