In this study, the catalytic efficiency of amorphous {Mo₇₂Fe₃₀} nanocapsules as a safe Keplerate polyoxometalate in organic synthesis was exploited. The easy-made solid catalyst exhibited high efficiency using a very low dosage (0.02–0.05 mol%) in the catalyzed condensation of various aromatic 1,2-diamines and aldehydes for the aerobic synthesis of benzimidazoles with very small E-factor values (0.11–0.33). The superior catalytic activity of amorphous nanoclusters compared to that of its crystalline counterpart was demonstrated. The high activity and recyclability of heterogeneous catalysts in a green reaction media under oxygen atmosphere, make this environmentally benign organic process appropriate for our applied goals.