In this work, the surface of mesoporous MCM-41 was modifed with guanidine, and then, Nickel particles have become immobilized on its surface (Ni-guanidine@MCM-41NPs). This heterogeneous catalyst has been identifed by various techniques including: low-angle X-ray difraction, scanning electron microscopy, energy-dispersive X-ray spectroscopy, inductively coupled plasma, thermal gravimetric analysis and N2 adsorption–desorption measurement isotherms, and its catalytic application was studied in the synthesis of 4,4ʹ-(arylmethylene)-bis-(3-methyl-1-phenyl-1H-pyrazol-5-ol) derivatives and symmetric di-aryl sulfdes. The prepared organometallic complex could be isolated, post-reaction, by simple fltration for several consecutive cycles without a notable change in its catalytic activity.