HIGHLIGHTS • Controllable and large-scale practical growth of plasmonic Ag-decorated vertically aligned 2D MoS 2 nanosheets on graphene. • Realization of the synergistic effects of surface plasmon resonance and favorable graphene/MoS 2 heterojunction to enhance the photoelectrochemical reactivity of 2D MoS 2. ABSTRACT A controllable approach that combines surface plasmon resonance and twodimensional (2D) graphene/MoS 2 heterojunction has not been implemented despite its potential for efficient photoelectrochemical (PEC) water splitting. In this study, plasmonic Ag-decorated 2D MoS 2 nanosheets were vertically grown on graphene substrates in a practical large-scale manner through metalorganic chemical vapor deposition of MoS 2 and thermal evaporation of Ag. The plasmonic Ag-decorated MoS 2 nanosheets on graphene yielded up to 10 times higher photo-to-dark current ratio than MoS 2 nanosheets on indium tin oxide. The significantly enhanced PEC activity could be attributed to the synergetic effects of SPR and favorable graphene/2D MoS 2 heterojunction. Plasmonic Ag nanoparticles not only increased visible-light and near-infrared absorption of 2D MoS 2 , but also induced highly amplified local electric field intensity in 2D MoS 2. In addition, the vertically aligned 2D MoS 2 on graphene acted as a desirable heterostructure for efficient separation and transportation of photo-generated carriers. This study provides a promising path for exploiting the full potential of 2D MoS 2 for practical large-scale and efficient PEC water-splitting applications.

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