wileyonlinelibrary.comcarbonization in a given atmosphere and hydrothermal carbonization are two promising techniques to accomplish the conversion from cellulose to carbonaceous materials. [ 12,13 ] Despite the fact that carbon structures form after releasing non-carbon atoms during the carbonization process, the conductivity of carbonized cellulose material is still low. [14][15][16] One strategy to enhance the conductivity of carbonized materials is to improve the graphitic structure of the carbonized product by increasing the carbonization temperature, which is also called graphitization. This stage enhances the order of the graphene stacks. [ 13 ] Graphitization is usually carried out at temperatures higher than 900 °C. A conductivity of 100 S/cm is obtained when the carbonization temperature is higher than 2000 °C; [ 17 ] however, such high temperatures require expensive equipment and are energy consuming.Chemically exfoliated graphene oxide (GO) is a twodimensional (2D) material, with rich hydroxyl, carboxyl, and epoxide functional groups on the basal planes and the planar edges. [ 18 ] It has been reported that GO may act as a template to assemble materials, to form novel structures or even to alternate molecular confi gurations. [19][20][21][22] Carbonization of GO fi lled poly(acrylonitrile) (PAN) nanofi bers demonstrates that GO can function as a template to improve the graphitic order and orientation in PAN carbon nanofi bers. [ 23 ] Studies also show that adding a very small amount of GO to glucose results in more conductive carbonized materials with higher degree of carbonization. [ 24 ] Thick layers of reduced GO (rGO) sheets are obtained, which is different from the spherical particles obtained from carbonization of pure cellulose. Such phenomena suggest that GO can be used as a template for cellulose carbonization. In addition, GO is a low cost building block to make highly conductive microfi bers. rGO microfi bers with a conductivity of 570 S/cm and 416 S/cm have been reported to be formed by chemical reduction and thermal reduction, respectively. [ 25,26 ] For the fi rst time, we reported highly conductive microfi bers based on GO and nanofi brillated cellulose (NFC) with GO serving as a template for cellulose carbonization, and carbonized NFC repairing the defects of carbonized/reduced GO (rGO) and linking rGO sheets together. Figure 1 a-b show the morphology change of NFC from fi bers to spherical particles after carbonization. In the carbonized GO+NFC (c(GO+NFC)) microfi bers, only Microfi bers with conductivity of 649 ± 60 S/cm are introduced through a carbonization of well-aligned graphene oxide (GO) -nanofi brillated cellulose (NFC) hybrid fi bers. GO acts as a template for NFC carbonization, which changes the morphology of carbonized NFC from microspheres to sheets while improving the carbonization of NFC. Meanwhile, the carbonized NFC repairs the defects of reduced GO (rGO) and links rGO sheets together. The GO templated carbonization of NFC as well as the alignment of the building block...