We report a novel nanostructured organosalt, based on sulfonic acid functionalized pyrazinium {[H-pyrazine–SO3H]Cl2} that was synthesized and characterized by several techniques including Fourier transform infrared (FT-IR) spectroscopy, X-ray diffraction (XRD), thermal gravimetric analysis (TGA), differential thermal gravimetric (DTG) analysis, transmission electron microscopy (TEM), mass spectrometry (MS), proton NMR (1H NMR), carbon-13 NMR (13C NMR) and also electron diffraction (ED) patterns. Results proved that the unprecedented sulfonated pyrizinium organosalt is indeed nanostructured and highly crystalline as supported by TEM, ED and XRD studies, having an average nanoparticle size of 50 nm according to TEM micrographs. The novel nano-organocatalyst was proved to be an efficient catalyst in the synthesis of 1,2,4,5-tetrasubstituted imidazoles by a one-pot multi-component condensation of benzil, a broad range of aldehydes, primary amines and ammonium acetate at 90 °C under solvent-free conditions.