Layered Ni(II) complex on magnetic nanoparticle as heterogeneous, efficient, novel, green, and reusable catalyst was used to cross‐coupling reaction, including carbon–carbon, carbon–nitrogen, and carbon–oxygen formations. The covalent functionalization of organic ligand, thiocarbohydrazide (TCH), on the surface of magnetic nanoparticle (Fe3O4) was determined that leading to an exceptional adsorptive ability for supporting Ni(II). The magnetic nano‐composite was characterized and investigated by using Fourier‐transform infrared spectroscopy (FT‐IR), thermogravimetric analysis (TGA), energy dispersive X‐ray (EDX), X‐ray diffraction (XRD), scanning electron microscope (SEM), inductively coupled plasma–optical emission spectrometry (ICP‐OES), transmission electron microscopy (TEM), and Brunauer–Emmett–Teller (BET). Also, three cross‐coupling reactions in the presence of Fe3O4@TCH@Ni(II) were optimized in terms of temperature, amount of catalyst, solvent, and time.