Low-cost methods for measuring airborne microparticles and nanoparticles (aerosols) have remained elusive despite the increasing concern of health impacts from ambient, urban, and indoor sources. While bipolar ion sources are common in smoke alarms, this work is the first to exploit the mean charge on an aerosol resulting from a bipolar charge equilibrium and establish experimentally its correlation to properties of the aerosol particle size distribution. The net current produced from this mean particle charge is demonstrated to be linearly proportional to the product of the mean particle diameter and total number concentration (i ∼ Nd̅) for two bipolar ion sources (85Kr and 241Am). This conclusion is supported by simple equations derived from well-established bipolar charging theory. The theory predicts that the mean charge on the aerosol particles reaches an equilibrium, which, importantly, is independent of the concentration of charging ions. Furthermore, in situ measurements of a roadside aerosol demonstrate that the sensing method yields results in good agreement (R2 = 0.979) with existing portable and laboratory-grade aerosol instruments. The simplicity, stability, and cost of the bipolar ion source overcome challenges of other portable sensors, increasing the feasibility of widespread sensor deployment to monitor ultrafine particle characteristics, which are relevant to lung deposition and by extension, human health.