In this work, a hierarchical reinforcement strategy for APCNs is presented. APCNs typically display better mechanical properties when compared to conventional hydrogels due to the presence of both hydrophilic and hydrophobic chain segments. Adding a peptidic hydrophobic phase provides a first level of reinforcement, while the HCNCs provide an additional mode to tune reinforcement. The main properties of the APCNs were studied to analyze the effect of the CNCs.