Highlights •Using 2D bimetallene for the composite lithium anode might be an efficient way to mitigate the growth of lithium dendrites.•Systematical first-principles calculations were performed to investigate the properties of Li deposition and diffusion on ten bimetallenes.•AgMn and AgPt bimetallenes were screened out as the anode candidates with high-performance to regulate the uniform lithium deposition.•AIMD simulations reveal that the strong interactions between Li metal with bimetallene would be beneficial to suppressing the growth of lithium dendrites.