Meng‐hui Wang, Zhengxuan Wang, Hao-lin Song, Guangtao Wang, Zhong‐hua Cui
Realizing topological superconductors (TSCs) with high transition temperatures (high- T c ) remains a central challenge in the development of fault-tolerant quantum computation. Here, we propose a route for realizing high- T c TSCs by integrating multigap superconductivity with nontrivial band topology in lithium-doped bilayer borophene. Extensive structural searches and high-throughput screening of over 4000 Li 1– x B x nanosheets identify eight promising multigap TSC candidates. Among them, the LiB 12 nanosheet is identified as a prototypical three-gap superconductor and simultaneously a topological metal with a symmetry-protected Dirac nodal loop. Fully anisotropic Migdal–Eliashberg calculations reveal cooperative couplings between σ↔in-plane and π↔out-of-plane phonon, which markedly enhance electron–phonon interactions and drive a high- T c of 57 K. These findings underscore the potential of metal-doped bilayer borophenes as a cutting-edge material platform for achieving high- T c multigap TSCs.