In this research, an innovative silica-based nanocomposite was designed and successfully manufactured. This nanomaterial, namely [SiO2@Si-pr-Bipyr-pr-Si@SiO2][FeCl4][HSO4] (SPBPSFH), was comprehensively analyzed using multiple techniques, including energy dispersive X-ray spectroscopy (EDS) for elemental composition verification, elemental mapping for distribution assessment of constituent elements, FT-IR for identification of functional groups and chemical bonds, scanning electron microscopy (SEM) for analysis of surface morphological features and determination of particles sizes, and X-ray diffraction (XRD) for crystallinity identification. SPBPSFH demonstrated remarkable activity in promoting the environmentally benign, solvent-free fabrication of 3,4-dihydropyrimidin-2(1H)-ones; the reaction was performed via the one-pot multi-component condensation of urea, aryl aldehydes and ethyl acetoacetate. Impressively, this catalytic system yielded the mentioned compounds in high to excellent yields, ranging from 90% to 98%. Furthermore, these outstanding results were achieved within relatively short reaction times of merely 30 to 50 min, underscoring the process efficiency. Notably, the catalyst demonstrated good recyclability and could be efficiently recovered and reused for three consecutive cycles without any significant loss of its catalytic activity.