Sketching a proper catalytic system with supplementary attributes, containing easy separation, wide surface area, supreme loading capacity, and fantastical electronic attributes, proposes an encouraging direction for efficiently using nanostructures for various applications. However, the capability to adjust the nano‐measure bimetallic particles is an adjustment for attaining superb performance in the catalytic field. Herein, an environmentally benign approach was developed for immobilizing and anchoring Pd‐Cu alloy nanoparticles on murexide (MX)‐functionalized carbon nanotubes (CNTs). Afterward, the catalytic activity of Pd2‐Cu3@MX/CNT was studied in synthesizing 2,3‐dihydro quinazoline‐4(1H)‐ones and carbon–carbon coupling reactions at sustainable reaction conditions under ultrasound irradiation. The results demonstrated that high‐affinity MX ligand and porous CNT structures than the adsorption of Pd–Cu had a unique designation in the high‐range constancy of the alloy nanoparticles and following catalytic activity. In addition, ultrasound irradiation got electrons of Pd–Cu alloy nanoparticles agitated, constructing a synergic efficacy between Cu and Pd metals for synthesis and coupling reactions. Our study represents that the designed catalyst is green, recyclable, and most suitable, providing new intuition into in high‐range constancy of bimetallic nanoparticles for broad applications.