In order to better understand nanostructured fiber networks, effects from high specific surface area of nanofibers are important to explore. For cellulose networks, this has so far only been achieved in nonfibrous regenerated cellulose aerogels. Here, nanofibrillated cellulose (NFC) is used to prepare high surface area nanopaper structures, and the mechanical properties are measured in tensile tests. The water in NFC hydrogels is exchanged to liquid CO2, supercritical CO2, and tert-butanol, followed by evaporation, supercritical drying, and sublimation, respectively. The porosity range is 40-86%. The nanofiber network structure in nanopaper is characterized by FE-SEM and nitrogen adsorption, and specific surface area is determined. High-porosity TEMPO-oxidized NFC nanopaper (56% porosity) prepared by critical point drying has a specific surface area as high as 482 m(2) g(-1). The mechanical properties of this nanopaper structure are better than for many thermoplastics, but at a significantly lower density of only 640 kg m(-3). The modulus is 1.4 GPa, tensile strength 84 MPa, and strain-to-failure 17%. Compared with water-dried nanopaper, the material is softer with substantiallly different deformation behavior.