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Cathode design is indispensable for building Li-O2 batteries with long cycle life. A composite of carbon-wrapped Mo2C nanoparticles and carbon nanotubes is prepared on Ni foam by direct hydrolysis and carbonization of a gel composed of ammonium heptamolybdate tetrahydrate and hydroquinone resin. The Mo2C nanoparticles with well-controlled particle size act as a highly active oxygen reduction reactions/oxygen evolution reactions (ORR/OER) catalyst. The carbon coating can prevent the aggregation of the Mo2C nanoparticles. The even distribution of Mo2C nanoparticles results in the homogenous formation of discharge products. The skeleton of porous carbon with carbon nanotubes protrudes from the composite, resulting in extra voids when applied as a cathode for Li-O2 batteries. The batteries deliver a high discharge capacity of ≈10 400 mAh g−1 and a low average charge voltage of ≈4.0 V at 200 mA g−1. With a cutoff capacity of 1000 mAh g−1, the Li-O2 batteries exhibit excellent charge-discharge cycling stability for over 300 cycles. The average potential polarization of discharge/charge gaps is only ≈0.9 V, demonstrating the high ORR and OER activities of these Mo2C nanoparticles. The excellent cycling stability and low potential polarization provide new insights into the design of highly reversible and efficient cathode materials for Li-O2 batteries. [ABSTRACT FROM AUTHOR]