Abstract Aluminum–Sulfur (Al–S) batteries are regarded as promising energy storage devices due to their high energy‐to‐price ratios and safety. However, they suffer from clumsy S ↔ Al 2 S 3 reactions and short lifespans that limit their practical application. By combining the merits of adsorptive Cu, catalytic Co, and conductive N‐doped carbon matrix, the bimetals decorated N‐doped carbon (Cu 1 Co 1 @NC) enables smooth adsorption and conversion of polysulfides. Consequently, the S@Cu 1 Co 1 @NC exhibits excellent electrochemical performance (delivering a high capacity of 317.5 mAh g −1 after 320 cycles at 1.5 A g −1 ). Moreover, the Cu‐endowed strong Al affinity and robust 3D scaffold with Co‐enhanced conductivity can regulate Al 3+ depositing/stripping and successfully suppress Al dendrites. As a result, the Cu 1 Co 1 @NC displays negligible Al nucleation overpotential and provides ultra‐long lifespan (>10 000 h) and exceptional reversible (Coulombic efficiency = 99.8–99.9%) Al 3+ plating/stripping. Integrating all these advantages, a full Al–S cell constructed with Cu 1 Co 1 @NC as two‐in‐one hosts demonstrates excellent capacity retention with enhanced reversibility. This work provides insights into the design of promising Al–S batteries based on bifunctional CuCo bimetal and favorable 3D framework.