in such areas. [2] The ideal efficiency of solar energy conversion of plasmonic metalbased hybrid catalysts comes from anisotropic crystallization, heterointerface. [3] Besides the morphology of plasmonic metal nanocrystals (NCs), the solar energy conversion efficiency of plasmonic metalsemiconductor NCs should be sensitive to the manner of coupling between metal NCs and the semiconductor. [4] Therefore, it is highly desirable to explore a versatile strategy to synthesize accurately controlled anisotropic configuration, monocrystalline shell, and intended site-selective heterocontact between plasmonic metal and semiconductor.The absorbance range is an essential factor on the efficiency of light harvesting and photoelectric catalysis. So far, most of the applications based on plasmonic metal hybrid NCs are limited in specific spectral range, because most of plasmonic metal nanostructures only have plasmon resonances in the visible regions. [5] Au nanorods (NRs), [6] because of its intriguing longitudinal surface plasmon resonance (LSPR), can be excited by incident light polarized along the axial direction. Therefore, it can be synthetically tailored across a broad spectral range and In this communication, light harvesting and photoelectrochemical (PEC) hydrogen generation beyond the visible region are realized by an anisotropic plasmonic metal/semiconductor hybrid photocatalyst with precise control of their topology and heterointerface. Controlling the intended configuration of the photocatalytic semiconductor to anisotropic Au nanorods' plasmonic hot spots, through a water phase cation exchange strategy, the site-selective overgrowth of a CdSe shell evolving from a core/shell to a nanodumbbell is realized successfully. Using this strategy, tip-preferred efficient photoinduced electron/hole separation and plasmon enhancement can be realized. Thus, the PEC hydrogen generation activity of the Au/CdSe nanodumbbell is 45.29 µmol cm −2 h −1 (nearly 4 times than the core/shell structure) beyond vis (λ > 700 nm) illumination and exhibits a high faradic efficiency of 96% and excellent stability with a constant photocurrent for 5 days. Using surface photovoltage microscopy, it is further demonstrated that the efficient plasmonic hot charge spatial separation, which hot electrons can inject into CdSe semiconductors, leads to excellent performance in the Au/CdSe nanodumbbell.The ORCID identification number(s) for the author(s) of this article can be found under https://doi.org/10.1002/aenm.201803889.Including the visible light (400-700 nm), the light harvest beyond visible (λ > 700 nm with ≈43% ratio of solar energy) to contribute effective photocatalysis is important but rarely studied. [1] Plasmonic metal based anisotropic metal-semiconductor hybrid nanostructures emerge to be potential materials for applications