Nanocomposites made from Na-montmorillonite and metallo-supramolecular polyelectrolytes (MEPE) based on nickel and ditopic bis-terpyridine ligands are prepared by an aqueous synthesis. Intercalation is confirmed by IR-spectroscopy, thermogravimetric analysis, and X-ray powder diffraction. The rheological response in the presence of an electric field of the dispersed nanocomposites in silicone oil is measured with a rheometer. The nanocomposites show a distinct electrorheological effect depending on the concentration and the kind of intercalated species. The effect occurs with a low content of active material while only very small currents are observed.