A novel hybrid nanomagnetic dendrimer-based catalyst was synthesized in this study using trimesoyl chloride and diethylene triamine as building blocks. Various characterization techniques, including FTIR, XRD, TGA, VSM, BET, SEM, and EDX, confirmed the successful construction of the nanostructure. The first-generation magnetic nanodendrimer catalyst (Fe₃O₄@SiO₂@DETA-TMD-G1) was used to synthesize Pyrano[3,2-c] chromene-3-carbonitrile derivatives in an aqueous medium. This method enhanced product yield (80–96%) and eliminated harmful organic solvents, making the process more sustainable. The catalyst also exhibited excellent magnetic recyclability, maintaining its efficiency over five consecutive reaction cycles. The presence of functionalized dendritic moieties enhanced efficient molecular interactions, leading to improved reaction rates, excellent yields, and higher selectivity for the desired heterocyclic products. By following green chemistry principles, this approach introduces a highly efficient, magnetically recoverable, and environmentally friendly catalytic system, offering a sustainable alternative for the synthesis of biologically active compounds with applications in pharmaceuticals and materials science