Catalytic decomposition of methane (CDM) is emerging as an efficient, greenhouse gas emission-free path for hydrogen production. This study demonstrates the notable performance of bimetallic Fesingle bondNi catalysts in CDM. Incorporating nickel into an iron-based catalyst significantly enhances methane conversion and hydrogen yield, with the benefit of producing valuable carbon nanotubes (CNT) as a byproduct. The 40Fesingle bond5Ni catalyst exhibits remarkable performance with 86 % methane conversion. A kinetic model is proposed; the removal of the first hydrogen atom from methane is the rate-determining step following its molecular adsorption on the catalyst surface. Additionally, catalyst deactivation is observed to follow first-order kinetics, with progressive accumulation of carbon deposits leading to a decline in catalytic activity over time. Furthermore, systematic DFT calculations reveal that Fesingle bondNi alloying shifts the d-band center, strengthening intermediate adsorption and enhancing methane decomposition for efficient hydrogen production. Overall, Fesingle bondNi bimetallic catalysts emerge as a cost-effective, scalable solution for sustainable hydrogen production, enabling carbon-neutral energy from methane.