This research explored the impact of four different electrolytes on the orientation of cellulose nanocrystals (CNCs) in shear-cast films prepared from aqueous CNC gels. Changes in the aqueous CNC gels’ rheological properties with electrolyte addition were correlated to the orientation and optical properties of dried CNC films. Film alignment was qualitatively assessed using cross-polarized optical microscopy and quantified by order parameters computed by UV–Vis transmission spectroscopy. Electrolyte addition resulted in an increased alignment in dried CNC films. For pure CNCs, the film order parameters remained constant at approximately 0.3 for shear rates from 20 s−1 to 100 s−1. However, higher order parameters were achieved in the presence of electrolytes. Notably, an order parameter of 0.88 was achieved at a shear rate of only 20 s−1. In addition, films produced from dispersions containing electrolytes exhibited improved clarity and haze. The results of this work highlight that electrolyte addition can enable higher order parameters at lower shear rates and facilitate the development of aligned CNC films for applications such as polarizers, clear coatings, and piezoelectric materials.
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