The active catalytic materials in stable inorganic supports are increasingly developing for the creation of ultra-stable catalysts with excellent performance. Here, the ZnO was supported on the surface of ZSM-5-type zeolite using Convolvulus persicus extract as a mild, efficient, cost‐effective, and eco‐friendly approach. The structure of the synthesized nanocatalyst was characterized using different techniques including UV, FT-IR, XRD, FE-SEM, EDS/Map, TGA, BET, and ICP-OES. The application of the ZnO/ZSM-5 as a catalyst was investigated in the Biginelli reaction between urea/thiourea, ethyl acetoacetate, and various aldehydes. Based on the results, ZnO/ZSM-5 exhibited good catalytic behavior, and the products were produced in excellent yields (90–95 %) in EtOH. This catalyst has notable benefits such as easy recovery and reusability (at least for five consecutive runs), simple work‐up, and high product yields.
