In this paper, TMU-3 with the general formula [HDMA]2[Zn2(BDC)3(DMA)2] 6DMF as a type of metalorganic framework materials (MOFs) was employed as a support for palladium nanoparticles to preparation a reusable heterogeneous catalyst with high performance (Pd@TMU-3). The Pd@TMU-3 catalyst was synthesized through a simple impregnation procedure and ion exchange of cations HDMA+ and Pd2+ in the TMU-3 and then was characterized by FT-IR, XRD, BET, FE-SEM, ESD-MAP, TGA, TEM, and ICPOES. Based on the results, Pd@TMU-3 with 1.3 mol %loading of Pd exhibited excellent efficiency in the Sonogashira coupling reaction between phenylacetylene and aryl halides with both electron-donor and electron-acceptor groups, and the products were produced good to excellent yields. The heterogeneous nanocatalyst can be a promising candidate in green chemistry due to its high catalytic performance in a short reaction time, high purity of products, recoverability, facile preparation, and easy transfer, which can notably decrease the costs as well as possible pollutions.