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Proton conducting nanocomposite solid polymer electrolytes (NSPEs) based on polyvinyl alcohol/ammonium nitrate (PVA/NH4NO3) and different contents of zinc oxide nanoparticles (ZnO-NPs) have been prepared using the casting solution method. The XRD analysis revealed that the sample with 2 wt.% ZnO-NPs has a high amorphous content. The ionic conductivity analysis for the prepared membranes has been carried out over a wide range of frequencies at varying temperatures. Impedance analysis shows that sample with 2 wt.% ZnO-NPs has a smaller bulk resistance compared to that of undoped polymer electrolyte. A small amount of ZnO-NPs was found to enhance the proton-conduction significantly; the highest obtainable room-temperature ionic conductivity was 4.71 × 10−4 S/cm. The effect of ZnO-NP content on the transport parameters of the prepared proton-conducting NSPEs was investigated using the Rice–Roth model; the results reveal that the increase in ionic conductivity is due to an increment in the number of proton ions and their mobility.