Magnetic particles were prepared by a hydrothermal method and then successively covered by Metal–Organic-Frameworks MIL-101-NH2 with a high surface area. This was followed by deposition of Pd(OAc)2 on Fe3O4–NH2@MIL-101-NH2 particles. The final catalyst was characterized with FT-IR, nitrogen physisorption, thermogravimetry (TGA), scanning electron microscopy (SEM) combined with energy dispersive X-ray analysis (EDX), transmission electron microscopy (TEM), vibrating sample magnetometry (VSM), wide-angle X-ray diffraction spectroscopy (XRD) and X-ray photoelectron spectroscopy (XPS). The prepared magnetic catalyst was effectively used in the Heck coupling reaction in the presence of an inorganic base. The reaction parameters such as the base type, amounts of catalyst and solvents, temperature, and substrates ratios were optimized. The catalyst was then magnetically separated, washed, and reused 7 times without losing significantly catalytic activity.