Strengthening the interaction between the substrate and the expensive transition metals such as palladium and increasing the capability of supporting in order to suppress the possibility of metal leaching from the surface is a very serious challenge in the design of a new heterogeneous catalyst. In this work, we develop the covalent functionalization of carboxylic ligand, ethylenediaminetetraacetic acid (EDTA), on the surface of the metal–organic framework of TMU-16-NH2, resulting in unparallel adsorptive ability for supporting Pd2+. The catalytic activity and stability of the synthesized catalyst named TMU-16-NH2-EDTA@Pd were studied in the Suzuki coupling reaction. We indicated that functionalization with EDTA plays a crucial role in boosting the adsorption capability of Pd and subsequently catalytic performance. The catalyst showed good reusability and has a nature truly heterogeneous due to the negligible leaching of palladium from the TMU16-NH2-EDTA@Pd surface.