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Li3BN2 is investigated for the first time as a transition metal free, high capacity cathode material for Li‐ion batteries. It is shown that α‐Li3BN2 can exhibit a specific capacity of 890 mA h g−1 with the charge storage mechanism associated with the valence state change of N ions in the BN2 anion. The specific capacity demonstrated in this study is the highest one ever reported in literature for an intercalation‐type cathode material. Further, using the valence state change of N ions as a charge storage mechanism opens the door for designing additional high performance, transition metal free electrodes in the future.

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