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Conversion of carbon dioxide (CO2) into useful chemicals is an important and urgent task from the energy and environment perspective. Herein, through a post-synthetic modification (PSM) approach, we synthesized three new metal–organic frameworks (MOFs) UiO-68-PSMs with different functional groups, namely, UiO-68-F, UiO-68-CH3 and UiO-68-OCH3, for the photocatalytic reduction of CO2. By introducing electron-withdrawing and electron-donating groups, UiO-68-PSMs showed different performance for the selective photocatalytic reduction of CO2 to CO because of change in charge separation and band gap of UiO caused by the presence of different functional groups. [ABSTRACT FROM AUTHOR]