relative low theoretical capacity of graphite anode (372 mAh g −1 ) hinders the development of LIBs with higher energy density. [2] Therefore, exploiting anode materials with high capacity are drawing increasing attention. [3] Alloying anode materials, such as Si, Sn, and Al, show great potential due to their high theoretical capacity (4200 mAh g −1 as Li 4.4 Si for Si, [4] 990 mAh g −1 as Li 4.4 Sn for Sn, [5] and 2235 mAh g −1 as Li 2.25 Al for Al [6] ). Particularly, Al is a promising candidate anode due to its excellent conductivity, high theoretical capacity, low discharge potential, natural abundance, and especially low cost. [7] However, Al-based anodes are usually investigated in half cells or full cells with low cathode areal density (<2 mg cm −2 ), which are far from practical requirements. [8] For example, Al-based anodes, such as thin film, [9] nanowires, [10] yolk-shell nanoparticles, [6b] Al-Si-graphite composite, [11] and Al/C hybrid nanoclusters, [12] were paired with Li metal to assemble half cells. Even though core-shell Al@C nanospheres, [13] Al foil, [14] carbon coated porous Al foil, [6a] and bubble sheet-like interfacial layer protected Al foil [15] were reported as anode in full cells with excellent cycling stability, the reported areal density of cathodes were very low (1-2 mg cm −2 ). In practical application, it is still a challenge to maintain the structural stability of Al-based anodes when they are paired with high areal density of cathode materials (>5 mg cm −2 ) in a full cell. [16] But, the cathode with high areal density means high areal capacity, and which results in severe volume expansion and pulverization of Al anode. The decay of anode would destroy the integrity, and accelerate the failure of the full battery. [17] Recently, we found that the cracking and pulverization of the Al battery could be attributed to the uneven charge/discharge reaction along the boundaries of pristine Al ( Figure S1a,b, Supporting Information), which lead to the stress concentration and ultimate failure of Al anode ( Figure S1c, Supporting Information). Therefore, it is possible to extend the lifetime of Al anode via uniform distribution of the alloying/dealloying stress. Herein, we report an inactive (Cu)/active (Al) nanocomposite design to achieve homogeneous reaction of Al anode. When the as-prepared Cu-Al-modified Al (namely Cu-Al@Al) anode Aluminum (Al) is one of the most attractive anode materials for lithium-ion batteries (LIBs) due to its high theoretical specific capacity, excellent conductivity, abundance, and especially low cost. However, the large volume expansion, originating from the uneven alloying/dealloying reactions in the charge/ discharge process, causes structural stress and electrode pulverization, which has long hindered its practical application, especially when assembled with a high-areal-density cathode. Here, an inactive (Cu) and active (Al) codeposition strategy is reported to homogeneously distribute the alloying sites and disperse the stress of volume expans...