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The rational regulation of geometry and dimension of plasmonic metal/semiconductor photocatalysts is crucial to optimize their photocatalytic performance by maxing the plasmonic effect. Herein, Au/CuSe/Pt hybrids with a tangential structure and strong dual‐plasmon resonance are prepared, for the first time, through a convenient hydrothermal method, which display a prominent photocatalytic hydrogen generation activity from water splitting. In the ternary nanostructure, a 2D CuSe ultrathin nanoplate is grown along the tangent of Au nanospheres, and Pt nanoparticles are deposited on Au and CuSe. Under visible and near‐infrared (VIS–NIR) light irradiation, the Au/CuSe/Pt hybrids exhibit an outstanding photocatalytic hydrogen generation activity, that is, 7.8 and 9.7 times that of Au/CuSe and Pt/CuSe, respectively. In an Au/CuSe/Pt nanosystem, CuSe and Au are both plasmonic units for light harvesting and near‐field enhancement, and Pt is cocatalyst for hydrogen reaction. Numerical simulations verify that Au and CuSe have strong electric field coupling around their interface, which can improve the abilities of light trapping and charge generation. Moreover, the closely contacted components and tangential architecture of Au/CuSe/Pt hybrids can generate multiple electron‐transfer pathways and abundant surface‐active sites, which arrestingly enhance the utilization of dual‐plasmon‐induced hot electrons and photoexcited charges, thus boosting hydrogen generation. [ABSTRACT FROM AUTHOR]

Plasmonic hybrids are regarded as promising candidates for water purification due to their structure-dependent photocatalysis and photothermal performance. It remains a challenge to develop materials that possess these two characteristics for efficient water purification. Herein, plasmonic Ti 3 C 2 T x /Bi 2 S 3 two-dimensional (2D)/2D hybrids were prepared for efficient solar-driven water purification via the combination of photothermal conversion and photocatalysis. Benefitting from broad light absorption, large 2D/2D interfaces, and efficient charge transfer, the binary hybrids showed high-efficiency photothermal conversion and photothermal-assisted photocatalytic activity. By depositing these 2D/2D hybrids on a hydrophilic and porous cotton piece, the Ti 3 C 2 T x /Bi 2 S 3 membrane displayed a high water evaporation rate and solar-to-vapor efficiency under one-sun irradiation. The solar-driven evaporation of seawater, heavy metal ion solution, and dye solution jointly indicated that the plasmonic membrane shows great potential for drinkable water generation and industrial wastewater treatment. Most importantly, the synergistic effect of photothermal evaporation and photocatalysis of the Ti 3 C 2 T x /Bi 2 S 3 membrane on water purification was demonstrated. The polluted water can not only be treated by evaporation, but also be degraded via photocatalysis under solar light irradiation. This work provides new insight into designing functional materials for water purification based on the combination of photothermal conversion and photocatalysis.