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Owing to the low‐cost, safety, and three‐electron redox properties of aluminum, rechargeable aluminum‐ion batteries (AIBs) are emerging as a promising energy storage technology. However, exploring suitable cathode material with both elevated working voltage and high reversible capacity remains a daunting challenge. Herein, under the guidance of density functional theory calculations, V6O13 is proposed as a promising cathode candidate in AIBs for the first time. It is demonstrated that aluminum ions are reversibly stored in V6O13 by intercalation reactions, with a high discharge voltage plateau of ≈1.1 V. Of particular note a pre‐lithiation strategy is employed to further promote the redox kinetics, which endows the pre‐lithiated V6O13 nanobelt (Li–VONB) with improved capacity of 161.6 mAh g−1 and impressive energy density of 177.7 Wh kg−1 after 300 cycles, far higher than other reported oxide cathodes in AIBs. Moreover, the shielding effect of pre‐inserted Li and accelerated diffusion rate are uncovered at the atomic scale. This work develops a novel Li–VONB cathode for high‐energy AIBs, and shows the great potential of pre‐intercalation strategies in the application of AIBs. [ABSTRACT FROM AUTHOR]