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A convenient method for the synthesis of pyrido[2,3‐d]pyrimidines by using the novel nano‐magnetic silica‐bonded S‐sulfonic acid[Fe3O4@SiO2@(CH2)3S–SO3H] as an efficient and recyclable catalyst under neat conditions is described. The major advantages of the present methodology are high yield, short reaction time, and reusability of the catalyst. Furthermore, the nano‐magnetic silica‐bonded S‐sulfonic acid was fully characterized by using various techniques such as FT‐IR, TG/DTG, DTA, EDX, μXRF, XRD, HRTEM, SEM, SEM elemental mapping, XPS, and N2 physisorption. The results obtained from this research support the idea of rational design, synthesis, and applications of task‐specific and reusable catalysts for the preparation of various polynitrogenated heterocyclic compounds containing 1,4‐dihydropyridine moieties.

A convenient multicomponent reaction towards the synthesis of natural henna‐based 3‐methyl‐1,4‐diphenyl‐1,4‐dihydrobenzo[6, 7]chromeno[2, 3‐c]pyrazole‐5,10‐dione derivatives by using a crabby nano glycoluril tetrakis(methylene phosphorous acid) (GTMPA), as an efficient and recyclable catalyst, under neat conditions is described. The major advantages of the synthetic methodology herein described are high yields, short reaction times, and the reusability of the catalyst, which has been fully characterized by Fourier Transform Infrared Spectroscopy (FT‐IR), Solid Phosphorus Nuclear Magnetic Resonance (31P NMR), Mass spectra (MS), X‐Ray Diffraction (XRD), High Resolution Transmission Electron Microscopy (HRTEM), Scanning Electron Microscope (SEM‐Mapp.), Energy Dispersive X‐Ray (EDX), Thermo Gravimetric Analysis (TGA), Differential Thermal Analysis (DTG), Differential Thermal Analysis (DTA) and X‐Ray Photoelectron Spectroscopy (XPS). The described biological‐based glycoluril with phosphorous acid pending may be applicable for the synthesis of gels, gelators, self‐healing and smart hydrogels.

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