Due to the importance and applicability of the catalysts in the oil, automobile, pharmaceutical, polymer, and food industries, they are one of the important links between basic sciences and applied technology with new technologies. Nanocatalysts are more efficient and more active than homogeneous catalysts, and operate in milder conditions. They also have a higher selectivity. The ZnS-ZnFe2O4 magnetic nanocatalyst was synthesized for the first time by a simple procedure, and was characterized using energy-dispersive X-ray spectroscopy (EDAX), field emission scanning electron microscopy (FESEM), X-ray diffraction analysis (XRD), and vibrating sample magnetometer (VSM). Then, it was used for the efficient synthesis of 1, 2-disubstituted benzimidazole derivatives using 1, 2-diamines and various aldehydes in ethanol. This heterogeneous catalyst can be recovered easily and reused without any significant loss of the catalytic activity. The present methodology offers several advantages such as high yields of products, shorter reaction time, and use of environmentally-friendly solvent.