The spontaneous motion of a nitrobenzene droplet on an Au electrode during an Sn electrodeposition has been reported in a previous paper (Chemphyschem, 9, 2302(Chemphyschem, 9, (2008). It also mentions that the velocity of the motion increases with a negative shift in the electrode potential. This present work has studied the motive force inducing the droplet motion, which is the imbalance between interfacial tension acting on the opposite side of a nitrobenzene droplet. As explained in the previous study, a high interfacial tension on the front side of the droplet is caused by an occurrence of electrodeposition. From this study, a low interfacial tension on the rear side has been found to attribute to an occurrence of hydrogen evolution reaction on the electrode surface. The rate of hydrogen evolution reaction increases as the electrode potential decreases, and thus the increase in the droplet velocity with a decreasing potential can be ascribed to the increase in the rate of hydrogen evolution reaction. The present work also reports that the velocity also increases by the addition of a salt such as K 2 SO 4 to the solutions. Wetting properties of solid surfaces are of interest from the viewpoint of interaction between liquid and solid phases. They play important roles not only in industrial processes but also in human activities. The wettability of a solid surface can be characterized by the contact angle of a liquid droplet on the solid surface.1,2 Figure 1 illustrates cross sections of oil droplets placed on solid surfaces in water (aqueous) phases. The contact angle of the droplet (θ) is defined by the mechanical equilibrium at the interface under the action of three interfacial tension (see Figure 1a), i.e., interfacial tension of solidwater interface (γ SW ), that of the solid-oil interface (γ SO ), and that of the oil-water interface (γ OW ), as expressed in the following Young's equation.1,2Comprehensive studies have demonstrated that a liquid droplet on a solid surface moves spontaneously due to an imbalance of interfacial tension acting on the droplet, as summarized in literatures. 2,3 As for an oil droplet on a solid surface in a water phase, the difference of γ SW between the front and rear sides of the droplet generates a driving force for the droplet to move spontaneously in the direction of a high interfacial tension, i.e., toward the region of higher wettability, as illustrated in Figure 1b.In the early 1990s, Ondarçuhu and Veyssie studied the behavior of a liquid droplet that was deposited on a boundary line between hydrophilic and hydrophobic parts of a plate. 4 The droplet moved spontaneously toward the region of higher wettability, and then stopped when the rear side of the droplet reached the boundary line. Chaudhury and Whitesides reported a spontaneous droplet motion induced by a wettability gradient on a solid surface.5 They generated a surfacechemical gradient on a silicon wafer surface by exposing it to the diffusing front of a vapor of decyltrichlorosilane.Since their studies were r...