Simultaneously increasing the activity and stability of the transition metal-based catalysts is critical for nonprecious metal catalysts toward oxygen reduction reaction (ORR). Herein, FeCo alloy nanoparticles encapsulated in nitrogen-doped carbon (NC) materials with surface-dangling M-N x active sites were fabricated, and the corresponding electrocatalytic performance was carefully investigated toward ORR in both alkaline and acid media. The coexistence of M-N x active species (Co 5.47 N or FeN 0.0324 ) and FeCo alloy makes the ORR reactivity strongly enhanced compared to the counterparts with only M-N x or FeCo species. Density functional theory calculations clearly reveal that the synergistic effect between FeCo, Fe-N x , and NC can induce the hybridization effect between d orbitals of Fe/Co and p orbitals of N/C atoms, and thus favor the desorption of *OH intermediates. Therefore, the FeN 0.0324 -FeCo@NC nanocatalyst with abundant mesopores and macropores shows enhanced electrocatalytic performance in both media (E 1/2 are 0.86 and 0.74 V, respectively).