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Plasmon-induced hot-electron transfer from metal nanostructures is being intensely pursed in current photocatalytic research, however it remains elusive whether molecular-like metal clusters with excitonic behavior can be used as light-harvesting materials in solar energy utilization such as photocatalytic methanol steam reforming. In this work, we report an atomically precise Cu13 cluster protected by dual ligands of thiolate and phosphine that can be viewed as the assembly of one top Cu atom and three Cu4 tetrahedra. The Cu13H10(SR)3(PR’3)7 (SR = 2,4-dichlorobenzenethiol, PR’3 = P(4-FC6H4)3) cluster can give rise to highly efficient light-driven activity for methanol steam reforming toward H2 production.