In this research, a novel nanostructured mesoporous organic-inorganic hybrid material, based on dicationic ionic liquid-anchored with silica, namely nano-2-[N′,N′-dimethyl-N′-(silica-n-propyl)ethanaminium chloride]-N,N-dimethylaminium bisulfate {nano-[DSPECDA][HSO4]} has been prepared, and characterized by FT-IR, energy-dispersive X-ray spectroscopy (EDX), field emission scanning electron microscopy (FE-SEM), X-ray diffraction (XRD), thermal gravimetry (TG), differential thermal gravimetric (DTG), differential thermal analysis (DTA), and adsorption/desorption porosimetry (BET, Langmuir, adsorption/desorption isotherm, BJH, and t-plot) methods. Thereafter, the nanomaterial has been utilized as a highly effectual, heterogeneous and recyclable nanocatalyst for the synthesis of N,N′-alkylidene bisamides via the condensation reaction of arylaldehydes (1 eq.) with primary amides (2 eq.) under solvent-free conditions. The reaction results were better compared with the literature in terms of two or more of these factors: turnover frequency (TOF), yield, temperature, time, and the reaction media. Moreover, a plausible mechanism for the synthesis has been proposed.