resources. [1][2][3][4][5] However, because of the slightly higher standard electrode potential of sodium (−2.7 V vs the standard hydrogen electrode (SHE)) than lithium (−3.02 V vs SHE), high-capacity electrode materials are needed for SIBs to compensate for their lower operation voltage and to achieve energy densities comparable to those of LIBs. It can be assumed that the cost of SIBs can be lowered relative to that of LIBs because of the cost-effectiveness of sodium resources. [6] These factors encourage us to explore potential highenergy-density cathode materials for SIBs.Among the various crystal structures of Na-containing compounds, layered structures have been intensively investigated because of their high capacity delivered under moderate operation conditions. The related layered structures are classified as O3, P2, P3, etc., according to the stacking sequence of the transition metals and alkali ions. [7][8][9] Layered sodium transition metal oxides of the form Na x MO 2 (M = Mn, Fe, Co, Ni, Cr, etc.) are stable in the P2 structure for Na contents (x) in the range of 0.3-0.7. This structure enables sodium ion diffusion between the two face-sharing trigonal prismatic sites such that P2-type layered materials generally exhibit higher discharge capacities than other layered materials. [10][11][12][13][14][15][16][17][18] Na 0.67 MnO 2 is one of the most common compounds among P2-type materials. [19][20][21][22][23] It delivers a high discharge capacity of over 175 mAh g −1 but exhibits severe capacity fade during cycling. One of the main reasons for this capacity fade is the structural disintegration caused by the Jahn-Teller effect of Mn 3+ ions in the MnO 6 octahedra, with elongation of the Mn 3+ -O distance along one direction. This Jahn-Teller effect can be mitigated by increasing the overall Mn oxidation state by substituting Mn with other elements, such as Ni, Co, Fe, Mg, and Al. [24][25][26][27][28][29] For example, improved cyclability was achieved in Mg-substituted Na 0.67 Mn 1−x Mg x O 2 (0.0 ≤ x ≤ 0.2) by suppressing the electrochemical activity of the Jahn-Teller Mn 3+ ions; however, this improvement was attained at the expense of the specific capacity. [26] Recently, Yabuuchi et al. [27] introduced a high-capacity P2-type Na 2/3 [Mg 0.28 Mn 0.72 ]O 2 material that exhibited capacities of over 150 mAh g −1 on charge and 220 mAh g −1 on discharge by raising the upper voltage cut-off to 4.6 V. Note that the average oxidation state of Mn in the compound is ≈3.85+, meaning that it cannot exhibit such a high charge capacity. The A high-rate of oxygen redox assisted by cobalt in layered sodium-based compounds is achieved. The rationally designed Na 0.6 [Mg 0.2 Mn 0.6 Co 0.2 ]O 2 exhibits outstanding electrode performance, delivering a discharge capacity of 214 mAh g −1 (26 mA g −1 ) with capacity retention of 87% after 100 cycles. High rate performance is also achieved at 7C (1.82 A g −1 ) with a capacity of 107 mAh g −1 . Surprisingly, the Na 0.6 [Mg 0.2 Mn 0.6 Co 0.2 ]O 2 compound is able to deliver...