Immobilization and heterogenization of acidic/basic groups or organic tags on inorganic supports have found many important applications in recent years. In this investigation, a new hybrid organic–inorganic nanostructure was prepared. The structure of novel nanomaterial was characterized by Fourier transform infrared spectroscopy, X-ray difraction, thermogravimetric analysis, vibrating sample magnetometer, scanning electron microscopy and the energy-dispersive X-ray spectroscopy techniques. The spirocompounds, especially spiroperimidines and pyranopyrazoles, are important structures with diverse biological activities and many applications in industries. So, the prepared hybrid nanomaterial was used as an efcient catalyst in the one-pot, green and simple protocol for the synthesis of pyranopyrazole, spiropyranopyrazole and spiroperimidine derivatives. The structure of some compounds is characterized by FT-IR, 1H-NMR and 13C-NMR analyses. In addition, the proposed intermediates were synthesized and identifed to prove the presented mechanism of the reaction. This hybrid nanomaterial is a recyclable and highly efcient heterogeneous catalyst and easily separated by an external magnet from the reaction media. The short reaction time, high efciency, operational safety and use of environmentally benign solvent are some benefts of this procedure.