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Abstract Lithium‐ion and sodium‐ion batteries (LIBs and SIBs) are crucial in our shift toward sustainable technologies. In this work, the potential of layered boride materials (MoAlB and Mo₂AlB₂) as novel, high‐performance electrode materials for LIBs and SIBs, is explored. It is discovered that Mo₂AlB₂shows a higher specific capacity than MoAlB when used as an electrode material for LIBs, with a specific capacity of 593 mAh g⁻¹achieved after 500 cycles at 200 mA g⁻¹. It is also found that surface redox reactions are responsible for Li storage in Mo₂AlB₂, instead of intercalation or conversion. Moreover, the sodium hydroxide treatment of MoAlB leads to a porous morphology and higher specific capacities exceeding that of pristine MoAlB. When tested in SIBs, Mo₂AlB₂exhibits a specific capacity of 150 mAh g⁻¹at 20 mA g⁻¹. These findings suggest that layered borides have potential as electrode materials for both LIBs and SIBs, and highlight the importance of surface redox reactions in Li storage mechanisms.