Natural photosynthetic systems use enzymes to split water, such as [Fe Fe]-hydrogenases with an active center consisting of a butterfly Fe₂S₂ cluster. Developing of artificial catalyst with similar, active center structure and functions is still one of main objectives in photocatalyst study for energy storage and conversion. In the present study, we prepared Fe₂S₂ nanocluster with doped Ni which possess similar active center to the center in [FeFe]-hydrogenases (the similar Fe-Fe bond length (2.60 Å), Fe-S-Fe bond angle and mbssbauer effect) for water splitting. Electrochemical measurements showed that the catalyst exhibited low onset potential about 30 mV and overpotential of ～0.12 V at 10 mA/cm² for hydrogen generation. Besides, by fabricated an artificial gill, Ni-doped Fe₂S₂ composite (AG-NFG) photocatalytic system performed significant enhanced activity for H₂ generation from pure water under visible light irradiation (λ ≥ 420 nm) without the use of sacrificial reagents.