Cellulose nanocrystals (CNCs), produced by the acid hydrolysis of wood, cotton or other cellulose-rich sources, constitute a renewable nanosized raw material with a broad range of envisaged uses: for example, in composites, cosmetics and medical devices. The intriguing ability of CNCs to self-organize into a chiral nematic (cholesteric) liquid crystal phase with a helical arrangement has attracted significant interest, resulting in much research effort, as this arrangement gives dried CNC films a photonic band gap. The films thus acquire attractive optical properties, creating possibilities for use in applications such as security papers and mirrorless lasing. In this critical review, we discuss the sensitive balance between glass formation and liquid crystal self-assembly that governs the formation of the desired helical structure. We show that several as yet unclarified observations—some constituting severe obstacles for applications of CNCs—may result from competition between the two phenomena. Moreover, by comparison with the corresponding self-assembly processes of other rod-like nanoparticles, for example, carbon nanotubes and fd virus particles, we outline how further liquid crystal ordering phenomena may be expected from CNCs if the suspension parameters can be better controlled. Alternative interpretations of some unexpected phenomena are provided, and topics for future research are identified, as are new potential application strategies.

Mechanically responsive textiles have transformative potential in many areas from fashion to healthcare. Cholesteric liquid crystal elastomers have strong mechanochromic responses that offer attractive opportunities for such applications. Nonetheless, making liquid crystalline elastomer fibres suitable for textiles is challenging since the Plateau–Rayleigh instability tends to break up precursor solutions into droplets. Here, we report a simple approach that balances the viscoelastic properties of the precursor solution to avoid this outcome and achieve long and mechanically robust cholesteric liquid crystal elastomer filaments. These filaments have fast, progressive and reversible mechanochromic responses, from red to blue (wavelength shift of 155 nm), when stretched up to 200%. Moreover, the fibres can be sewed into garments and withstand repeated stretching and regular machine washing. This approach and resulting fibres may be useful for applications in wearable technology and other areas benefiting from autonomous strain sensing or detection of critically strong deformations.

We review the research on carbon nanotube (CNT) dispersion in liquid crystals (LCs), focusing mainly on the approaches where the aim is to align CNTs along the LC director field, but also covering briefly the proposed possibility to enhance thermotropic LCs by CNT doping. All relevant LC types are considered: thermotropic LC hosts allowing dynamic CNT realignment, lyotropic LC hosts allowing very high concentration of CNTs uniformly aligned over macroscopic areas and consequent removal of the LC, and LC phases formed by CNTs themselves, used in spinning high-quality carbon nanotube fibres. We also discuss the issue of CNT dispersion in some detail, since successful nanotube separation is imperative for success in this field regardless of the type of LC that is considered. We end by defining a few major challenges for the development of the field over the next few years, critical for reaching the stage where industrially viable protocols for LC-based CNT alignment can be defined.

The packing of cellulose nanocrystals (CNC) in the anisotropic chiral nematic phase has been investigated over a wide concentration range by small-angle X-ray scattering (SAXS) and laser diffraction. The average separation distance between the CNCs and the average pitch of the chiral nematic phase have been determined over the entire isotropic–anisotropic biphasic region. The average separation distances range from 51 nm, at the onset of the anisotropic phase formation, to 25 nm above 6 vol % (fully liquid crystalline phase) whereas the average pitch varies from ≈15 μm down to ≈2 μm as ϕ increases from 2.5 up to 6.5 vol %. Using the cholesteric order, we determine that the twist angle between neighboring CNCs increases from about 1° up to 4° as ϕ increases from 2.5 up to 6.5 vol %. The dependence of the twisting on the volume fraction was related to the increase in the magnitude of the repulsive interactions between the charged rods as the average separation distance decreases.