In this study, we are interested in preparing Fe(III), Pd(II), and Cu(II) complexes from new thiazole derivatives. All syntheses were elaborately elucidated to estimate their molecular and structural formulae, which agreed with those of mononuclear complexes. The square-planer geometry of Pd(II) complex (MATYPd) was the starting point for its use as a heterocatalyst in preparing pyrazole-4-carbonitrile derivatives 4a–o using ultrasonic irradiation through a facile one-pot reaction. The simple operation, short-time reaction (20 min), and high efficiency (97%) were the special advantages of this protocol. Furthermore, this green synthesis strategy was advanced by examination of the reusability of the catalyst in four consecutive cycles without significant loss of catalytic activity. The new synthesis strategy presented remarkable advantages in terms of safety, simplicity, stability, mild conditions, short reaction time, excellent yields, and use of a H₂O solvent. This catalytic protocol was confirmed by the density functional theory (DFT) study, which reflected the specific characteristics of such a complex. Logical mechanisms have been suggested for the successfully exerted essential physical parameters that confirmed the superiority of the Pd(II) complex in the catalytic role. Optical band gap, electrophilicity, and electronegativity features, which are essential parameters for the catalytic behavior of the Pd(II) complex, are based mainly on the unsaturated valence shell of Pd(II).