The swelling of the HCNC_00 initially increased relative to the peptidic APCNs previously reported, but as the content of HCNCs increased, swelling in both water and n-hexane was reduced and remained constant independent of the content of HCNC. Nevertheless, the CNC-reinforced APCNs do swell in water and in n-hexane and are, therefore, hydrogels and lyogels. The Tg of the HCNC-P samples remained between 30 -36 °C. The TGA analysis shows a decrease in the degradation temperature with the addition of the peptides and the HCNCs. All the samples were transparent, which is a remarkable result given that high concentrations of CNCs could scatter light if the CNCs were not well dispersed in the polymer matrix. The optimal reinforcement of dry samples and samples swollen in n-hexane was obtained at HCNC concentrations between 6 and 15 wt%. For the samples swollen in water, reinforcement was observed for all the HCNC-peptidic samples. Therefore, HCNCs are a novel additive to reinforce APCNs. However, synthesis required the use of a solvent which has a slightly negative effect on the mechanical properties compared to peptide-reinforced APCNs which were synthesized with less solvent. This work highlights that CNCs can serve as an additional pathway to reinforce hierarchical APCNs while retaining the key material properties and enhancing the physical properties, thus allowing tailoring for different applications ranging from soft contact lenses, to biomaterials, and membranes.