Molybdenum　(Mo)　serves　as　the　key　site　in　the　nitrogenase　enzyme,　catalyzing　the　conversion　of　N2　into　NH3　under　ambient　conditions.　However,　the　strong　affinity　of　Mo　sites　for　N2　hinders　H2　adsorption　due　to　the　competitive　nature　of　N2　and　H2　on　a　single　site,　resulting　in　an　unsatisfactory　ammonia　synthesis　performance.　Here,　we　propose　an　approach　of　intervening　C60　layer　as　a　second　site　for　H2　adsorption　on　two-dimensional　Mo2CTx.　The　C60　layer　thickness　is　readily　tunable　by　varying　its　loading　content.　An　optimal　C60　layer　significantly　enhances　the　electronic　interaction　between　the　C60　layer　and　the　Mo2CTx　layer,　leading　to　a　remarkable　decrease　in　the　work　function　and　an　increase　in　the　electron　density　of　Mo　atoms.　Therefore,　the　separate　adsorption　of　N2　and　H2　on　distinct　sites　is　substantially　facilitated.　The　present　work　offers　insights　into　the　correlation　between　structure　and　performance　in　NH3　synthesis　catalysts.　©　2025　American　Institute　of　Chemical　Engineers.