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Abstract Coordination polymerization leads to various metal–organic frameworks (MOFs) with unique physical properties and chemical functionalities. One of the challenges towards their applications as porous materials is to make MOFs optimally conductive to be used as electronic components. Here, it is demonstrated that Co-MOF-74, a honeycomb nano–framework with one–dimensionally arranged cobalt atoms, advances its physical properties by accommodating tetracyanochinodimethan (TCNQ), an acceptor molecule. Strong intermolecular charge transfer reduces the optical band gap down to 1.5 eV of divalent TCNQ and enhances the electrical conduction, which allows the MOF to be utilized for resistive gas- and photo-sensing. The results provide insight into the electronic interactions in doped MOFs and pave the way for their electronic applications.