This study deals with the designing and preparation of PdII immobilized on ferromagnetic multi-walled carbon nanotubes functionalized by aminated 2-chloroethylphosphonic acid with S-methylisothiourea -FMMWCNTs@CPA@SMTU@PdII NPs- as a versatile ferromagnetic nanostructured catalyst. Fourier transform infrared -FT-IR-, X-ray diffraction -XRD- analysis, transmission electron microscopy -TEM-, field emission scanning electron microscopy -FE-SEM-, energy-dispersive X-ray spectroscopy -EDX-, EDS-map, thermogravimetric analysis -TGA-, vibrating sample magnetometry -VSM-, inductively coupled plasma atomic emission spectroscopy -ICP-OES- and X-ray photoelectron spectroscopy -XPS- were used to characterize the nanocatalyst. The results show that FMMWCNTs@CPA@SMTU@ PdII NPs with decorated MWCNTs by Fe3O4 NPs exhibited ferromagnetic properties with a uniform rod-like morphology and particle sizes of about 20–30 nm. The catalytic performance of FMMWCNTs@CPA@SMTU@PdII NPs was evaluated in Sonogashira- Hagihara cross-coupling reaction at room temperature and in solvent-free conditions. Under appropriate condition, all reactions proceeded at a faster initial rate while exhibiting excellent activity and selectivity and the desired products were obtained in relatively excellent yields.

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