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Atomically precise Ni 6 (SC 2 H 4 Ph) 12 nanoclusters (Ni 6 NCs) supported on g-C 3 N 4 nanosheets were constructed to enhance the photocatalytic hydrogen evolution performances. [Display omitted] Much effort has been devoted to improving the photocatalytic capacity of graphitic carbon nitride (g-C 3 N 4). In this paper, we reported the successful synthesis of a hybrid photocatalyst with superb photocatalytic hydrogen production activity through decorating atomically precise Ni 6 (SC 2 H 4 Ph) 12 nanoclusters on g-C 3 N 4 nanosheets (labeled as Ni 6 /g-C 3 N 4) at room temperature. Zeta potential experiments demonstrated that the electrostatic interaction between Ni 6 and g-C 3 N 4 led to the formation of Ni 6 /g-C 3 N 4. The photocatalytic measurements revealed that the 5 %-Ni 6 /g-C 3 N 4 prepared with the original mass ratio of m(Ni 6)/m(g-C 3 N 4) = 1/20 exhibited the strongest hydrogen production activity. In the system with triethanolamine (TEOA) as the sacrifice agent, the visible-light hydrogen production rate reached up to 5.87 mmol h−1 g−1, approximately 290 times higher than that of pure g-C 3 N 4 (0.02 mmol h−1 g−1). Density functional theory (DFT) calculations testified that the above significant enhancement of photocatalytic hydrogen evolution of the hybrid photocatalyst arose from the photogenerated electrons transfer from Ni 6 to g-C 3 N 4. [ABSTRACT FROM AUTHOR]