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Single-entity electrochemistry is of fundamental importance and shows promise for ultrasensitive biosensing applications. Recently, we have demonstrated that various charged nanoparticles can be detected individually based on the non-redox open-circuit potential (OCP) changes induced by their collision events on a floating carbon nanoelectrode (CNE). Unlike the widely used amperometry approach, the potentiometric method provides the label-free detection of individual nanoscale entities without redox mediators in the solution. However, the CNE lacks specificity for molecular recognition during the collision events because of the limited methods of surface functionalization for carbon surfaces. Herein, we used surface-functionalized gold nanoelectrode (GNE) to overcome this limitation of CNE. The GNE modified with Raman reporter molecule also enabled surface-enhanced Raman spectroscopy (SERS) measurements. By using simultaneous time-resolved OCP and SERS measurements, both the OCP and SERS signals induced by the “hit-n-run” type of gold nanoparticle (GNP) collision events can be better understood. Also, by introducing a zwitterionic molecule, we formed near “stealth” surface and demonstrated that the non-specific adsorptions of GNPs to the surface of GNE have been suppressed, allowing continuous detection of hit-n-run events for over 30 min.