Nanofibrillated
cellulose (NFC) has received increasing attention in science and technology
because of not only the availability of large amounts of cellulose
in nature but also its unique structural and physical features. These
high-aspect-ratio nanofibers have potential applications in water
remediation and as a reinforcing scaffold in composites, coatings,
and porous materials because of their fascinating properties. In this
work, highly porous NFC aerogels were prepared based on <i>tert</i>-butanol freeze-drying of ultrasonically isolated bamboo NFC with
20–80 nm diameters. Then nonagglomerated 2–20-nm-diameter
silver oxide (Ag<sub>2</sub>O) nanoparticles (NPs) were grown firmly
onto the NFC scaffold with a high loading content of ∼500 wt
% to fabricate Ag<sub>2</sub>O@NFC organic–inorganic composite
aerogels (Ag<sub>2</sub>O@NFC). For the first time, the coherent interface
and interaction mechanism between the cellulose I<sub>β</sub> nanofiber and Ag<sub>2</sub>O NPs are explored by high-resolution
transmission electron microscopy and 3D electron tomography. Specifically,
a strong hydrogen between Ag<sub>2</sub>O and NFC makes them grow
together firmly along a coherent interface, where good lattice matching
between specific crystal planes of Ag<sub>2</sub>O and NFC results
in very small interfacial straining. The resulting Ag<sub>2</sub>O@NFC
aerogels take full advantage of the properties of the 3D organic aerogel
framework and inorganic NPs, such as large surface area, interconnected
porous structures, and supreme mechanical properties. They open up
a wide horizon for functional practical usage, for example, as a flexible
superefficient adsorbent to capture I<sup>–</sup> ions from
contaminated water and trap I<sub>2</sub> vapor for safe disposal,
as presented in this work. The viable binding mode between many types
of inorganic NPs and organic NFC established here highlights new ways
to investigate cellulose-based functional nanocomposites