It is demonstrated that it is possible to coat the individual fibers of wood-based nanocellulose with polypyrrole using in situ chemical polymerization to obtain an electrically conducting continuous high-surface-area composite. The experimental results indicate that the high surface area of the water dispersed material, to a large extent, is maintained upon normal drying without the use of any solvent exchange. Thus, the employed chemical polymerization of polypyrrole on the microfibrillated cellulose (MFC) nanofibers in the hydrogel gives rise to a composite, the structure of whichunlike that of uncoated MFC paperdoes not collapse upon drying. The dry composite has a surface area of ∼90 m2/g and a conductivity of ∼1.5 S/cm, is electrochemically active, and exhibits an ion-exchange capacity for chloride ions of 289 C/g corresponding to a specific capacity of 80 mAh/g. The straightforwardness of the fabrication of the present nanocellulose composites should significantly facilitate industrial manufacturing of highly porous, electroactive conductive paper materials for applications including ion-exchange and paper-based energy storage devices.