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•Exfoliated nanosheets of conductive MOFs demonstrated outstanding activity and excellent selectivity in photocatalytic CO2 reduction.•Photogenerated electrons from sensitizer could be translocated and dispersed into the conductive MOFs with rich active sites.•The morphology, high dispersion of electrons and isolated Ni-N4 motifs synergically contribute to the excellent photocatalytic performance.
Mimicking the natural photosynthesis process, photocatalytic conversion of CO2 has been an ongoing hotspot of scientific research and technology development. A key aspect is the discovery of high potency catalysts for facilitating the multi-electron participated reactions. Herein we successfully demonstrate exfoliated nanosheets from a conductive 2D-MOF Ni3(HITP)2 as an efficient co-catalyst for CO2 reduction in a hybrid photocatalytic system under visible light illumination. By taking advantage of the high conductivity for charge transportation and highly accessible active sites for redox reactions, an excellent selectivity of 97% for deoxygenative CO2 reduction and a high CO yield rate of 3.45 × 104 μmol·g−1 h−1 were achieved with superior stability. This work provides essential insights into future design and development of more effective MOFs-based systems for catalytic CO2 utilization.