Simultaneous incorporation of cellulose
nanocrystals (CNCs) and
chitin nanofibers (ChNFs) into a polyvinyl alcohol (PVA) matrix opens
possibilities for customization of more environmentally friendly composite
materials. When used in tricomponent composite hydrogels, the opposite
surface charges on CNCs and ChNFs lead to the construction of beneficial
nanofiber structures. In this work, composite hydrogels containing
CNCs, ChNFs, or their mixtures are produced using cyclic freeze–thaw
(FT) treatments. When considering different compositions and FT cycling,
tricomponent composite hydrogels containing a specific ratio of CNCs/ChNFs
are shown to have promising mechanical performance in comparison to
other samples. These results together with results from water absorption,
rheological, and light scattering studies suggest that the CNC/ChNF
structures produced property improvement by concurrently accessing
the stronger interfacial interactions between CNCs and PVA and the
longer lengths of the ChNFs for load transfer. Overall, these results
provide insight into using electrostatically driven nanofiber structures
in nanocomposites.