Conductive metal–organic frameworks (c-MOFs) show great potential in electrochemical energy storage thanks to their high electrical conductivity and highly accessible surface areas. However, there are significant challenges in processing c-MOFs for practical applications. Here, we report on the fabrication of c-MOF nanolayers on cellulose nanofibers (CNFs) with formation of nanofibrillar CNF@c-MOF by interfacial synthesis, in which CNFs serve as substrates for growth of c-MOF nanolayers. The obtained hybrid nanofibers of CNF@c-MOF can be easily assembled into freestanding nanopapers, demonstrating high electrical conductivity of up to 100 S cm–1, hierarchical micromesoporosity, and excellent mechanical properties. Given these advantages, the nanopapers are tested as electrodes in a flexible and foldable supercapacitor. The high conductivity and hierarchical porous structure of the electrodes endow fast charge transfer and efficient electrolyte transport, respectively. Furthermore, the assembled supercapacitor shows extremely high cycle stability with capacitance retentions of >99% after 10000 continuous charge–discharge cycles. This work provides a pathway to develop flexible energy storage devices based on sustainable cellulose and MOFs.

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Novel nanosheets prepared by interweaving ZIF-67-templated LDH nanocrystals with nanocellulose and CNTs are applied in flexible and foldable energy storage devices.