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Summary of main observation and conclusion In order to extend the absorption spectrum of poiyoxo-titanium clusters into the visible region,two new heterometal-oxo clusters Ti4CuⅡ2CuⅠ2(μ3-O)6(benzoate)10(MeCN)4 (PTC-153) and Ti4CuⅡ2Cu12(μ3-O)6(benzoate)8(CH3COO)2(MeCN)4 (PTC-154) were successfully synthesized.Single-crystal X-ray diffraction and X-ray photoelectron spectroscopy studies showed that these two heterometallic Ti4Cu4-oxo clusters possessed Chinese knot-shape structure and mixed valence Cu1+/2+ ions.UV-visible spectroscopy analysis demonstrated that the visible light region absorption of PTC-153 and PTC-154 could be significantly enhanced by doping copper.Furthermore,their visible-light driven photocurrent responses were studied by using samples of PTC-153 and PTC-154 as electrode precursors.