Abstract In this study, Fe-Ni bimetallic catalyst supported on kaolin is prepared by a wet impregnation method. The effects of mass of kaolin support, pre-calcination time, pre-calcination temperature and stirring speed on catalyst yields are examined. Then, the optimal supported Fe-Ni catalyst is utilised to produce multi-walled carbon nanotubes (MWCNTs) using catalytic chemical vapour deposition (CCVD) method. The catalysts and MWCNTs prepared using the optimal conditions are characterized using high resolution transmission electron microscope (HRTEM), high-resolution scanning electron microscope (HRSEM), electron diffraction spectrometer (EDS), selected area electron diffraction (SAED), thermogravimetric analysis (TGA), Brunauer-Emmett-Teller (BET), and X-ray diffraction (XRD). The XRD/EDS patterns of the prepared catalyst confirm the formation of a purely crystalline ternary oxide (NiFe2O4). The statistical analysis of the variance demonstrates that the combined effects of the reaction temperature and acetylene flow rate predominantly influenced the MWCNT yield. The N2 adsorption (BET) and TGA analyses reveal high surface areas and thermally stable MWCNTs. The HRTEM/HRSEM micrographs confirm the formation of tangled MWCNTs with a particle size of less than 62 nm. The XRD patterns of the MWCNTs reveal the formation of a typical graphitized carbon. This study establishes the production of MWCNTs from a bi-metallic catalyst supported on kaolin.