This study investigates the role of Ni in CNT production using Fe-based catalysts. Among the various catalysts used, such as 40Fe-0Ni, 40Fe-1Ni, 40Fe-3Ni, 40Fe-5Ni, 40Fe-7Ni, and 40Fe-10Ni, the 40Fe-5Ni catalyst achieved a notable yield of 5.80 gC per g metal, which is higher than the 1.03 gC per g metal obtained with the pure Fe catalyst. DFT study reveals that Fe3Ni exhibits stronger carbon binding, enabling more efficient CNT production and supporting our experimental results.