The bilayer borophene has been successfully fabricated in experiments recently and possesses superior antioxidation and robust metallic properties, which holds great promise for the future anode materials of Li-ion batteries. Herein, using first-principles calculations, two bilayer borophenes including P6/mmm or P6̅ m2 symmetry groups with or without vacancy defects are comprehensively explored and acted as electrode materials with high performance in Li-ion batteries. The charge density difference, adsorption energies, and Bader charge analysis are calculated and discussed for single lithium adsorbed on bilayer borophene. The results shown that with the increase of lithium concentration, the adsorption energies are rapidly decreased due to the repulsion of boron atoms except for the P6̅ m2 systems with double side adsorption and corresponding energies remain the narrow range. Meanwhile, the partial density of states shows metallic character after lithium adsorption and indicates good conductivity for the charge−discharge process. Furthermore, small diffusion barriers, low average open-circuit voltage, can be achieved, and large storage capacity is up to 930.2 mA h/g at the lower lithium content of 0.375. These results propose that bilayer borophene might be a good choice for anode material applications in future Liion batteries with fast ion diffusion and high power density.