We have tackled in situ electric conductance measurements under microscopic observations for alignments of silica particles that are induced by ionic polarization of the electrical double layer (EDL) around the particles. Using the in situ conductance measurements, we have presented evidence that electro-osmotic flow at a vessel bottom/water interface would be coupled with the ionic polarization in the EDL of spherical silica particles settling at the bottom (Langmuir 2007, 23, 8797). In this study, we followed this phenomenon further. We altered the zeta potential of a platform of a glass plate on which a pearl chain of silica particles was formed under an ac electric field to control the mobility of electro-osmotic flow at the macroscopic interface of the platform/water. As the magnitude of the zeta potential of the platform increased, the surface distance between neighboring particles in the pearl chains decreased and the in situ conductance totally increased due to the enhancement of the dipole moments induced by the ionic polarizations of the particles. These results could be explained by considering that the electro-osmotic contribution to the surface conduction around the particles would be coupled with that occurring at the platforrn/water interface.