An attempt was made to synthesize novel composites comprising poly(2-hydroxyethyl methacrylate) (PHEMA) and cellulose nanocrystallites (CNC) (acid-treated cotton microfibrils) from suspensions of CNC in an aqueous 2-hydroxyethyl methacrylate (HEMA) monomer solution. The starting suspensions (similar to 5 wt % CNC) separated into an isotropic upper phase and an anisotropic bottom one in the course of quiescent standing. By way of polymerization of HEMA in different phase situations of the suspensions, we obtained films of three polymer composites, PHEMA-CNCiso, PHEMA-CNCaniso, and PHEMA-CNCmix, coming from the isotropic phase, anisotropic phase, and embryonic nonseparating mixture, respectively. All the composites were transparent and, more or less, birefringent under a polarized optical microscope. A fingerprint texture typical of cholesteric liquid crystals of longer pitch spread widely in PHEMA-CNCaniso but rather locally appeared in PHEMA-CNCiso. Any of the CNC incorporations into the PHEMA matrix improved the original thermal and mechanical properties of this amorphous polymer material. In dynamic mechanical measurements, the locking-in of the respective CNC assemblies gave rise to an increase in the glass-state modulus E' of PHEMA as well as a marked suppression of the E'-falling at temperatures higher than T-g (similar to 110 degrees C) of the vinyl polymer. It was also observed for the composites that their modulus E' rerose in a range of about 150-190 degrees C, which was attributable to a secondary cross-linking formation between PHEMA chains mediated by the acidic CNC filler. The mechanical reinforcement effect of the CNC dispersions was ensured in a tensile test, whereby PHEMA-CNCaniso was found to surpass the other two composites in stiffness and strength.