Graphite is a key cathode material for aluminum-ion batteries (AIBs), but appears poor structural stability and cyclability due to the slow kinetics of intercalation and usage of conductive additives. So far, reasonable design and construction of high-conductive, flexible, binder-free graphitic film cathodes with fast kinetics of anion intercalation mechanism still remains challenging for high-power and high-energy AIBs. Herein, we report the reasonable design for facile construction of high-conductive and mechanically flexible film cathode of high-quality few-layer graphene (FLG) nanosheets for high capacity and fast AIBs, thanks to the strong synergy of ionic surface adsorption/desorption of graphene and ionic intercalation/deintercalation of graphite. The FLG nanosheets prepared by electrochemical cathodic exfoliation from graphite, exhibit predominantly 3∼5 layers, extremely low I_D/I_G ratio of < 0.05, ultrahigh C/O atom ratio of 43, and excellent solution-processability, which allow for large-area production of highly conducting (1300 S cm^-1), binder-free and densely stacked FLG films as extremely stable cathodes for ultrafast AIBs. It’s worth mentioning that the resulting AIBs exhibit high capacity of 173 mAh g^-1 at 1 A g^-1, outstanding rate capability with exceptionally large capacity of 101 mAh g^-1 at 10 A g^-1 that outperforms the most reported graphitic materials, long-term cyclability without noticeable capacity loss after 10000 cycles, and good performance at wide range of temperatures. The multiple characterizations and theoretical simulation further confirm that the unique performance is attributed to the synergistic mechanisms of diffusion-controlled intercalation and surface adsorption of FLG film. Therefore, this work will open intriguing opportunities for the development of advanced AIBs.

石墨是铝离子电池（AIB）的关键阴极材料，但由于插层的动力学缓慢和使用导电添加剂，因此显示出较差的结构稳定性和可循环性。到目前为止，对于高功率和高能量的AIB，具有快速阴离子迁移机理的高导电性，柔性，无粘合剂的石墨膜阴极的合理设计和构造仍然具有挑战性。在此，由于离子表面吸附/解吸的强大协同作用，我们报告了用于高容量和快速AIB的高质量几层石墨烯（FLG）纳米片的高导电性和机械柔性膜阴极的简便结构的合理设计。石墨烯和石墨的离子嵌入/脱嵌。FLG纳米片是通过石墨的电化学阴极剥离制成的，_D / I _G比<0.05，超高C / O原子比为43，出色的固溶加工性能，可大面积生产高导电性（1300 S cm ^-1），无粘合剂和密集堆叠的FLG膜作为超快AIB的极稳定阴极。值得一提的是，所得AIB在1 A g ^-1时显示出173 mAh g ^-1的高容量，出色的速率能力，在10 A g ^-1时显示101 mAh g ^-1的超大容量其性能优于大多数报道的石墨材料，可长期循环使用，10000次循环后无明显容量损失，并且在宽温度范围内均具有良好的性能。多种表征和理论模拟进一步证实，独特的性能归因于扩散控制插层和FLG膜表面吸附的协同机制。因此，这项工作将为高级AIB的开发提供有趣的机会。