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The application of polyaniline nanofibers doped with chloride and nitrate ions (PANINFs-Cl and PANINFs-NO3) in potentiometry was described. Both kinds of nanofibers were used as an ion-to-electron transducer in ion-selective electrodes with solid contact (SCISEs). Extensive research on the properties of the nanofibers themselves (SEM, UV–Vis spectroscopy, FTIR) and the constructed electrodes (potentiometric methods, electrochemical impedance spectroscopy) has been carried out. Basic analytical parameters of electrodes containing various nanofibers contents in the ion-selective membrane and with nanofibers as an intermediate layer were determined. It was found that application of PANI nanofibers resulted in improvement of electrode performance (among others, better stability and reversibility of the electrode potential). The obtained sensors were characterized by a high slope of the calibration curve, a wide measuring range and a fast response time. Moreover, they were insensitive to change of redox potential, as well as light and the presence of oxygen in the solution, what is important from a practical point of view. They were also successfully used for nitrate determination in real environmental samples.