Bioinspired nanocomposites have attracted
considerable
attention
as robust, lightweight, and functional materials for various applications.
These bioinspired materials contain high fractions of reinforcements
and form highly ordered hard/soft nanocomposite structures with balanced
molecular interactions. Herein, we fabricate bioinspired ternary nanocomposites
of sodium carboxymethylcellulose (CMC) and polydopamine (PDA)-modified
cellulose nanocrystals (DCNCs) with bouligand-type architectures via
water-borne evaporation-induced self-assembly (EISA). The surfaces
of cellulose nanocrystals (CNCs) were coated with PDA polymer to improve
the interfacial adhesion between CNCs and CMC. We tune the structure
formation and material properties by using different feed ratios of
polymer-to-CNCs. Material properties were tailored further in ternary
nanocomposites by balancing CMC and PDA amounts within the total polymer
content at a given feed ratio. CMC–DCNC ternary nanocomposites
with higher CNC content exhibit better-ordered structures, synergistic
mechanical performances, and improved functional properties than CMC–CNC
binary nanocomposites. CMC–DCNC nanocomposites with 70 wt %
CNC loading show excellent mechanical strength (183 ± 36 MPa)
and stiffness (15 ± 0.5 GPa) at 20% relative humidity (RH), placing
these materials among the top-end of CNC-based bioinspired nanocomposites
reported so far. Due to the stable and efficient interfacial interactions
between DCNCs and CMC, ternary nanocomposites demonstrate comparatively
much higher mechanical properties than CMC–CNC and pristine
CMC films, even at higher RH (50 and 80% RH). Crack propagation studies
using field-emission scanning electron microscopy display different
crack growth and toughening mechanisms like crack deflection, layered
delamination, and microcrack generation, resulting in synergistic
mechanical improvement in the ternary nanocomposites. Due to the presence
of PDA, CMC–DCNC nanocomposites also exhibit higher thermal
stability, UV-shielding properties, free-radical scavenging ability,
and water vapor barrier properties, which are essential characteristics
for packaging materials. Thus, CMC–DCNC nanocomposites prepared
from sustainable building blocks using a bioinspired design strategy
show potential as robust, green, UV-protective films for food packaging.