of ions or charged particles. This instrument is able to distinguish analytes of different concentrations down to μm level. [2] Such features in detection enable the conductivity meter as a potential sensing platform. [9] Gold nanoparticles (AuNPs) have won a considerable attention because of their excellent properties such as low cost, good dispersity, controllable aggregation, and convenient surface modification. AuNPs have been widely used in detecting analytes including amino acids, nucleic acids, and even single molecules. [10,11] Most of these sensors are based on the modulation of dispersion and aggregation of AuNPs due to their unique surface plasmon resonance (SPR). The dispersed AuNPs present a red color and the aggregated AuNPs present a blue color. The introduction of targets can induce the aggregation of AuNPs that results in a change in the plasmon coupling between AuNPs. Accordingly, the absorption peak in the SPR spectrum shows a redshift. By means of the modulation from dispersion to aggregation, varieties of plasmonic assays have been designed. For example, cyclodextrin-functionalized AuNPs were directly used as optical probes for the determination of dopamine. [12] AuNPs modified with red blood cell membranes could assemble in the presence of fibrinogen. [13] Despite the straightforward readout, these AuNPs-based optical sensors require complicated surface modification or ligand exchange. [11] More importantly, the sensitivity of the colorimetric method can be an issue at a low concentration of analyte. The color change of AuNPs might be not effective for highly sensitive detection. Therefore, developing other readout methods for AuNPs-based detection can be beneficial for applications that require high sensitivity.Similar to ions, the free-moving AuNPs have conductivity that plays an important role in electrophoresis. [14] However, few studies focus on the EC value of AuNPs that might derive from the difficulty in explaining the intricate interparticle interactions and relative kinetics, such as the Brownian motion and aggregation. The EC property of AuNPs is determined by many factors that are closely interconnected. [15] For example, the concentration of AuNPs greatly affects the EC value. [16] Besides, the physical contact of AuNPs within an aggregated network facilitates the electron transportation that can increase the EC value. In addition, the relative thickness of the electrical double layer is vital to the EC value. [17] A thicker electrical double layer tends to increase the hydrated radius of AuNPs, leading to a reduced electrophoretic mobility and a decreased EC value. [18] Developing a versatile sensing toolkit with high sensitivity may revolutionize current techniques for analytical applications. This work reports a sensing strategy through the electrical conductivity of gold nanoparticles (AuNPs). By modulating the concentration, aggregation, and surface ligand of AuNPs, a versatile analytical platform for highly sensitive detection based on the electrical conductivity is outlin...