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For constructing next-generation lithium-ion batteries with advanced performances, pursuit of high-capacity Li-rich cathodes has caused considerable attention. So far, the low discharge specific capacity and serious capacity fading are strangling the development of Fe-based Li-rich materials. To activate the extra-capacity of Fe-based Li-rich cathode materials, a facile molten salt method is exploited using an al-kaline mixture of LiOH–LiNO3 –Li 2 O2 in this work. The prepared Li 1.09 (Fe 0.2 Ni 0.3 Mn 0.5 ) 0.91 O2 material yields high discharge specific capacity and good cycling stability. The discharge specific capacity shows an up-ward tendency at 0.1 C. After 60 cycles, a high reversible specific capacity of ～250 mAh g 1 is delivered. The redox of Fe 3 /Fe 4 and Mn 3 /Mn 4 are gradually activated during cycling. Notably, the redox reaction of Fe2 /Fe 3 can be observed reversibly below 2 V, which is quite different from the material prepared by a traditional co-precipitation method. The stable morphology of fine nanoparticles (10 0–30 0 nm) is considered benefiting for the distinctive electrochemical performances of Li 1.09 (Fe 0.2 Ni 0.3 Mn 0.5 ) 0.91 O2 . This study demonstrates that molten salt method is an inexpensive and effective approach to activate the extra capacity of Fe-based Li-rich cathode material for high-performance lithium-ion batteries.