Nanopores are emerging as a powerful tool for the analysis and characterization of nanoparticles at the single entity level. Here, we report that a polymer electrolyte nanopore system enables the enhanced detection of nanoparticle at low ionic strength when a PEG-based polymer electrolyte is present inside the nanopore. We developed a numerical model that recapitulates the electrical response of the nanopore system and the model revealed that the electrical response of the glass nanopore is sensitive to the position of the polymer electrolyte interface. As proof of concept, we demonstrated the multimodal analysis of a nanoparticle sample by coupling the polymer electrolyte nanopore sensor with nanoimpact electrochemistry. This combination of techniques could deliver the multiparametric analysis of nanoparticle systems complementing electrochemical reactivity data provided by nanoimpact electrochemistry with information on size, shape and surface charge provided by nanopore measurements.