Fuel cells are a very powerful renewable and clean energy technology, but their extensive applications are restricted because of the high cost and poor reliability of cathodic catalysts for oxygen reduction reaction (ORR). Herein, we report on highefficiency, low-cost, iron and nitrogen co-doped carbon sphere (Fe/NPCS) ORR electrocatalysts obtained by hydrothermal synthesis of 3-aminophenol−formaldehyde (APF) resin and subsequent pyrolysis. Both the Fe 3+ concentration and surfactant are modulated in the polymerization and cross-linking process under hydrothermal conditions, and their main effects on the morphology, specific surface area, and electrocatalytic aspects are evaluated. Upon optimization of the Fe feeding amounts, we obtained Fe/NPCSs-M with 0.33 at. % Fe, which exhibited excellent ORR catalytic performance. The electrochemical test showed that the onset and half-wave potentials of Fe/NPCSs-M were 0.92 and 0.78 V vs those of the reversible hydrogen electrode (vs RHE), respectively, which are comparable to those of commercial Pt/C catalysts (0.94 and 0.82 V), and the diffusion-limiting current density was 6.0 mA cm −2 , which is higher than that of Pt/C catalysts (5.6 mA cm −2 ). The oxygen reduction reaction involved a 4-electron transfer process under the catalysis of Fe/NPCSs-M, which is a very useful electron transfer path for ORR, and the byproduct H 2 O 2 yield was less than 4%. The methanol resistance and cycle stability of Fe/NPCSs-M were also better than those of Pt/C catalysts. Our results can help develop a very promising ORR catalyst and motivate further work into advanced nitrogencontaining resorcinol−formaldehydes for determining their electrocatalytic behavior.