LAUSR

Nickel (II) ions (Ni (II)) doped into the zinc‐based metal–organic framework Zn‐BDC have shown exceptional catalytic activity as heterogeneous catalysts for the three‐component Biginelli condensation reaction, delivering yields ranging from 62% to 96% with excellent selectivity under diverse reaction conditions. The Ni doping was achieved through a facile solvothermal synthesis, producing Ni(x)‐Zn‐BDC catalysts, where x represents the weight percentage of Ni relative to Zn (e.g., Ni[10]‐Zn‐BDC). Comprehensive characterization of the synthesized catalysts was conducted using advanced spectroscopic and analytical techniques, confirming successful incorporation of Ni into the Zn‐BDC framework without compromising its structural integrity. The Ni(10)‐Zn‐BDC catalyst, in particular, exhibited remarkable efficiency in facilitating the reaction under mild conditions. Furthermore, the catalyst demonstrated excellent recyclability and stability, maintaining consistent catalytic performance over multiple cycles. These findings highlight Ni(x)‐Zn‐BDC as a promising and sustainable material for the synthesis of dihydropyrimidinones, underscoring its potential in green and efficient catalytic processes.