Bulk of present day hydrogen comes from gasification of coal, steam reforming, and partial oxidation of hydrocarbons. Steam reforming accounts for over 50% of world hydrogen production despite producing carbonaceous gases which are harmful to the environment. In this work, five different supported molten metal catalysts comprising varying quantities of nickel and lithium supported on calcium oxide were synthesized and designated according to weight % as; 50%Ni/CaO, 37.5%Ni-12.5%Li/CaO, 25.0%Ni-25.0%Li/CaO, 12.5%Ni-37.5%Li/CaO, and 50%Li/CaO. The synthesized catalysts were characterized by scanning electron microscopy, X-ray diffraction, Brunauer-Emmett-Teller, and transmission electron microscopy and tested for methane decomposition. During decomposition experiments, the performance of each catalyst under different temperature conditions was evaluated in terms of methane conversion, carbon, and hydrogen yield. From experimental data obtained, catalyst 37.5%Ni-12.5%Li/CaO recorded 65.7% methane conversion and 38.3%hydrogen yield, while catalyst 50%Ni/CaO recorded the lowest methane conversion of 60.2% and a hydrogen yield of 35.7% at 650 C-degrees. This confirms that the molten environment aided catalyst activity in methane decomposition reaction.