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[Display omitted] • A novel dinuclear cobalt complex with definite structure was successfully synthesized and used as a cocatalyst in a photocatalyst H 2 production system. • This system exhibits an average H 2 evolution rate of 1045 μmol·h−1 within 8 h. • This system can work for 24 h with a TON of 16,400. Photocatalytic water splitting to produce hydrogen has gradually become a research hotspot in recent years, and molecular cocatalysts especially cobalt-based complexes as proton reduction cocatalysts have attracted wide attention due to their high activity and selectivity. In this study, CdS nanorods were employed as photosensitizers, and a novel dinuclear cobalt-bis(thiosemicarbazone) complex with definite structure was used as a cocatalyst to improve visible-light-driven hydrogen evolution. Under the optimum conditions, this noble metal-free system exhibited an average hydrogen evolution rate of 1045 μmol·h−1 in 8 h irradiation. This system could work for 24 h with a TON of 16,400, and the average apparent quantum yield of this system is ∼21% at 420 nm. On the basis of photoelectrochemical studies and electrochemical analysis, we proposed a possible mechanism for hydrogen production in this three-component system. [ABSTRACT FROM AUTHOR]