It is of significant implication to fabricate high-performance, durable and low-cost catalysts toward to oxygen reduction reaction (ORR) to drive commercial application of fuel cells. In our work, we synthesize the Fe/N-CNT catalyst via one-pot grinding combined with calcination using a mixture of carbamide, CNTs and iron salts as precursors, the as-synthesized catalysts show the structure that Fe nanoparticles are encapsulated in the tube of intertwined CNTs with abundant active sites. The catalyst is synthesized at 800 °C (Fe/N-CNT-800-20) obtain high graphitization degree and high N doped content, especially the high content and proportion of Fe-N and pyridinic-N, exhibiting outstanding ORR activity. Moreover, too high calcination temperature (850 °C) and high Fe content (25%) lead to the agglomeration of Fe during the calcination, which blocked some catalytic sites, leading to poor ORR activity. This facile synergy route will provide new thoughts for the fabrication and optimization of catalysts.