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In today's society, mankind is confronted with two major problems: the energy crisis and the greenhouse effect. Artificial photosynthesis can use solar energy to convert the greenhouse gas CO2 into high-value compounds, which is an ideal solution to alleviate the energy crisis and solve the problem of global warming. The combination of ZnO and polythiophenes (PTh) can make up for each other's drawbacks, thus improving the photoresponse behavior and separation efficiency of the photogenerated carriers. The PTh layer can transfer photogenerated electrons to ZnO, thereby extending the lifetime of the photogenerated charges. The production rate of CH4 from the photoreduction of CO2 with ZnO/PTh10 is 4.3 times that of pure ZnO, and the selectivity of CH4 is increased from 70.2% to 92.2%. The conductive PTh can absorb photons to induce π–π* transition, and the photogenerated electrons can transfer from the LUMO to the conduction band (CB) of ZnO, thus more electrons are involved in the reduction of CO2. [ABSTRACT FROM AUTHOR]