Ruthenium supported on oxides or on carbon is reported to have the highest ammonia cracking activity. Due to scarcity and high price of precious metal catalysts, abundant, low-cost alternatives are needed. Early transition metal carbides and nitrides uniquely exhibit catalytic properties similar to Pt-group metals due to partially filled d-orbitals and modified d-band structures. Our team develops unique Mo2C and Mo2N supported catalysts and tunes synergistic effects of metal-support interactions. Our work shows nickel on Mo2C to achieve higher H2 production rates than Ru and 5%Ru/Al2O3.