Metal-based catalysts play an essential role in organic chemistry and the chemical industry. This research designed and successfully synthesized a pillar-layered metal–organic framework (MOF) with the urea linkers, namely Basu-HDI, as a novel and efcient heterogeneous catalyst. Various techniques such as FT-IR, EDX, elemental mapping, SEM, XRD, BET, and TGA/DTA studied its structure and morphology. Then, we investigated the synthesis of new 1,8-naphthyridines utilizing Basu-HDI in mil conditions via a one‐pot, three‐component tandem Knoevenagel/Michael/ cyclization/anomeric-based oxidation reaction. Final products were achieved by anomeric-based oxidation without employing an oxidation agent. Remarkably, this tandem process gave a good range of new 1,8-naphthyridines with high yields in a short reaction time. The pure products were confrmed by FT-IR, H NMR, 13C NMR, and mass spectrometry techniques. Moreover, the introduced catalyst showed good efciency and stability and can be reused four times without signifcantly reducing efciency.