This article presents an experimental study, performed in the BERGAME setup, dedicated to studying the collection of submicron aerosol particles by raindrops. The initial aim was to focus on the influence of the electrical charges of raindrops on the efficiency with which they collect aerosol particles. However, in the relative humidity range considered in this article (26–36%), measurements highlight a first-order role of phoretic effect for submicron aerosol particles. Indeed, measurements highlight a 100% increase in the collection efficiency for each percentage decrease in the atmospheric relative humidity. Phoretic effects are known to play a role in collection by drops; however, none of the models found in the literature predicts the same magnitude as the one presently measured. Characterization of the aerosol trajectories around the drop, accelerated to terminal velocity, seems to show a coupling between phoretic effects and rear capture. This interaction, already suggested by Grover et al., is a line of explanation for such a sharp unpredicted increase of the collection efficiency with moisture decrease.