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An unprecedented {CuTe} core incorporated in a 36-tungsto-4-silicate polyoxometalate with visible light-driven catalytic hydrogen evolution activity.

We report an unprecedented {CuII14TeIV10} core containing the novel μ,μ-/μ6-TeIVO32- mode and TeIVO44- embedded within a 36-tungsto-4-silicate POT shell, which constitutes the first example of a tellurous copper cluster in POMs. The structure-stabilizing and templating effects of tellurite anions are crucial for this assembly. Moreover, its visible light-driven catalytic H2 evolution activity and related quenching mechanism are demonstrated, and extensive stability studies are presented.