Collagen (Col) hydrogels are an important biomaterial with many applications in the biomedical sector. However, deficiencies, including insufficient mechanical properties and a rapid rate of biodegradation, hamper their application. In this work, nanocomposite hydrogels were prepared by combining a cellulose nanocrystal (CNC) with Col without any chemical modification. The high-pressure, homogenized CNC matrix acts as nuclei in the collagen’s self-aggregation process. The obtained CNC/Col hydrogels were characterized in terms of their morphology, mechanical and thermal properties and structure by SEM, rotational rheometer, DSC and FTIR, respectively. Ultraviolet-visible spectroscopy was used to characterize the self-assembling phase behavior of the CNC/Col hydrogels. The results showed an accelerated assembling rate with the increasing loading of CNC. The triple-helix structure of the collagen was preserved with a dosage of CNC of up to 15 wt%. The CNC/Col hydrogels demonstrated an improvement in both the storage modulus and thermal stability which is attributed to the interaction between the CNC and collagen by the hydrogen bonds.