Fe-N-C catalysts are potential substitutes to displace electrocatalysts containing noble chemical elements in the oxygen reduction reaction (ORR). However, their application is hampered by unsatisfactory activity and stability issues. The structures and morphologies of Fe-N-C catalysts have been found to be crucial for the number of active sites and local bonding structures. In this work, dicyandiamide (DCDA) and polyaniline (PANI) are shown to act as dual nitrogen sources to tune the morphology and structure of the catalyst and facilitate the ORR process. The dual nitrogen sources not only increase the amount of nitrogen doping atoms in the electrocatalytic Fe-C-N material, but also maintain a high nitrogen-pyrrole/nitrogen-graphitic: (N-P)/(N-G) value, improving the distribution density of catalytic active sites in the material. With a high surface area and amount of N-doping, the Fe-N-C catalyst developed can achieve an improved half-wave potential of 0.886 V (vs. RHE) in alkaline medium, and a better stability and methanol resistance than commercial Pt/C catalyst.