Nanostructured materials are difficult to prepare rapidly and as large structures. The present study is thus significant because a rapid preparation procedure for large, flat, smooth, and optically transparent cellulose nanopaper structures is developed using a semiautomatic sheet former. Cellulose/inorganic hybrid nanopaper is also produced. The preparation procedure is compared with other approaches, and the nanopaper structures are tested in uniaxial tensile tests. Optical transparency and high tensile strength are demonstrated in 200 mm diameter nanopaper sheets, indicating well-dispersed nanofibrils. The preparation time is 1 h for a typical nanopaper thickness of 60 μm. In addition, the application of the nanopaper-making strategy to cellulose/inorganic hybrids demonstrates the potential for "green" processing of new types of nanostructured functional materials.