Although advances have been reported to mimic the mechanically excellent structure of natural nacre, larger-scale applications are still limited due to time and energy-intensive preparation pathways. Herein, we demonstrate that simple high-shear homogenization of dispersions containing biobased high molecular weight sodium carboxymethyl cellulose (700 kg/mol, CMC) and natural sodium montmorillonite (MTM), serving as the soft energy-dissipating phase and reinforcing platelets, respectively, can be used to prepare large-area and thick films with well-aligned hard/soft nacre-mimetic mesostructure. During this process, core–shell nanoplatelets with intrinsic hard/soft structure form, which then self-assemble into a layered nanocomposite during water removal. The nanoscale periodicities of the alternating hard/soft layers can be precisely tuned by changing the ratio of CMC to MTM, which allows studying the evolution of mechanical properties as a function of the lamellar nanoscale periodicity and fractions of hard to soft material. Remarkable mechanical stiffness (25 GPa) and strength (320 MPa) can be obtained placing these materials among the top end of nacre-inspired materials reported so far. Mechanical homogenization also allows direct preparation of concentrated, yet homogeneous, gel-like dispersions of high nanoclay content, suited to doctor-blade large-area and thick films with essentially the same properties as films cast from dilute dispersions. In terms of functional properties, we report high-transparency, shape-persistent fire-blocking and the ability to surface-pattern via inkjet printing. Considering the simple, fully scalable, waterborne preparation pathway, and the use of nature-based components, we foresee applications as ecofriendly, bioinspired materials to promote sustainable engineering materials and novel types of functional barrier coatings and substrates.