Nacre-mimicking hybrids of high inorganic content (>50 wt %) tend to show low strain-to-failure. Therefore, we prepared clay nanopaper hybrid composite montmorillonite platelets in a continuous matrix of nanofibrillated cellulose (NFC) with the aim of harnessing the intrinsic toughness of fibrillar networks. Hydrocolloid mixtures were used in a filtration approach akin to paper processing. The resulting multilayered structure of the nanopaper was studied by FE-SEM, FTIR, and XRD. Uniaxial stress-strain curves measured in tension and thermal analysis were carried out by DMTA and TGA. In addition, fire retardance and oxygen permeability characteristics were measured. The continuous NFC matrix is a new concept and provides unusual ductility to the nanocomposite, allowing inorganic contents as high as 90% by weight. Clay nanopaper extends the property range of cellulose nanopaper and is of interest in self-extinguishing composites and in oxygen barrier layers.