The ability to tune the bimetallic particles in nano-scale is essential for achieving high activities in the catalytic arena. This study reported a new strategy for anchoring and long-term stabilizing Pd–Ni alloy nanoparticles (NPs) with Pd: Ni mole ratios 2: 3 onto Kryptofix 23 (K23) functionalized SBA-15. Subsequently, the catalytic activity of Pd2–Ni3@K23/SBA-15 was developed in carbon-carbon, carbon-nitrogen, and carbon-oxygen coupling reactions under ultrasound irradiation. The findings indicated that porous SBA-15 structure and high-affinity K23 ligand toward adsorption of Pd–Ni had an outstanding role in the long-term stability of the alloy NPs and subsequent catalytic activity. Furthermore, electrons of Pd–Ni alloy NPs were excited by ultrasound irradiation and created a synergic effect between Pd and Ni metals for cross-coupling reactions. The proposed protocol was the greener, recyclable, and more suitable option for the large-scale application, providing some new insights into in long-term stability of bimetallic NPs.