A highly active iron-nitrogen-doped carbon nanotube catalyst for the oxygen reduction reaction (ORR) is produced by employing vertically aligned carbon nanotubes (VA-CNT) with a high specific surface area and iron(II) phthalocyanine (FePc) molecules. Pyrolyzing the composite easily transforms the adsorbed FePc molecules into a large number of iron coordinated nitrogen functionalized nanographene (Fe-N-C) structures, which serve as ORR active sites on the individual VA-CNT surfaces. The catalyst exhibits a high ORR activity, with onset and half-wave potentials of 0.97 and 0.79 V, respectively, versus reversible hydrogen electrode, a high selectivity of above 3.92 electron transfer number, and a high electrochemical durability, with a 17 mV negative shift of E-1/2 after 10 000 cycles in an oxygen-saturated 0.5 m H2SO4 solution. The catalyst demonstrates one of the highest ORR performances in previously reported any-nanotube-based catalysts in acid media. The excellent ORR performance can be attributed to the formation of a greater number of catalytically active Fe-N-C centers and their dense immobilization on individual tubes, in addition to more efficient mass transport due to the mesoporous nature of the VA-CNTs.