Increase in the water contact angle of composite film surfaces caused by the assembly of hydrophilic nanocellulose fibrils and nanoclay platelets.

Controlling the assembly modes of different crystalline nanoparticles in composites is important for the expression of specific characteristics of the assembled structures. We report a unique procedure for increasing water contact angles (CAs) of composite film surfaces via the assembly of two different hydrophilic components, nanocellulose fibrils and nanoclay platelets. The nanocellulose fibrils and nanoclay platelets used have ionic groups on their surfaces in high densities (∼1 mmol g(-1)) and have no hydrophobic surface. The increase in the CA of the nanocellulose/nanoclay composite films was thus analyzed on the basis of the air area fractions of their nanostructured surfaces following Cassie's law. The air area fractions were geographically estimated from the atomic force microscopy height profiles of the composite film surfaces. The CAs of the composite film surfaces were found to be well described by Cassie's law. Interestingly, the composite films consisting of two hydrophilic nanoelements with different shapes exhibited CAs larger than those of the individual neat films.