AbstractBackgroundAmides are the essential building blocks of natural products and bioactive molecules. One of the most common structures discovered in medicinal and bioactive compounds is amide derivatives. The synthesis of N‐(pyridin‐2‐yl)arylamide compounds has recently been assessed using various methods. In particular, there is growing interest in employing heterogeneous catalysts to catalyze organic synthesis reactions. Metal organic frameworks based on nickel centers were synthesized using the solvothermal method. The morphology, size, and catalytic activity of Ni‐based catalysts strongly depend on the substitute solvent composition in the reaction system. The structural features of the Ni‐based materials were verified using modern analytical techniques.ResultsNi‐based materials were used to catalyze the synthesis of physiologically important N‐(pyridin‐2‐yl)arylamides through an amidation reaction between 2‐aminopyridine and benzaldehyde. Temperature, reaction time, catalyst amount, reactant ratio, and solvent type were investigated as factors that influenced the catalytic activity. The optimal reaction conditions were 10 mol% Ni‐based catalysts, tetrahydrofuran as the reaction solvent, and a reaction temperature of 90 °C for 24 h. N‐(pyridin‐2‐yl)arylamide was obtained in approximately 85% yield. The catalyst could be recovered and reused without significant loss of catalytic activity (79%) after six runs.ConclusionThis study illustrated that the Ni‐based catalyst performed well in the reaction between 2‐aminopyridine and benzaldehyde formation N‐(pyridin‐2‐yl)arylamide compound with an 85% yield. The solid catalyst was recovered and reused up to six times without any significant change in catalytic activity. © 2023 Society of Chemical Industry (SCI).