Dual-atom Fe catalysts supported by three nitrogen atom doped graphene (Fe-TM/GP, where TM = Ti, V, Cr, Mn, Fe, Co, Ni, and Cu) are explored for methane adsorption and activation. The addition of the second metal significantly tunes the properties of the catalysts. The main factor influencing methane adsorption is electron transfer. The second metal promotes methane adsorption by altering the electronic properties such as the band structure and charge transfer. A volcano-shaped relationship is found between the absolute value of adsorption energy and energy barrier at the heteroatom Fe-TM/GP. Fe-Ni/GP has the lowest energy barrier. Heteroatom Fe-TM/GP has a lower energy barrier than Fe-Fe/GP.