Cellulose nanocrystals (CNXLs) have drawn attention from researchers for their remarkable reinforcing abilities and excellent mechanical properties. CNXLs typically have high aspect ratios of around 20-50 (length/width), low density of around 1.6 g/cc, high stiffness (135 to 155 GPa), and strength (estimated at 7500 MPa). Here we utilize CNXLs in a bottom-up hierarchical assembly to produce a macroscale material. Single-stranded oligonucleotides with an amino modifier were successfully grafted on CNXLs. The molecular recognition ability of the oligomeric base pairs was then utilized by duplexing complementary oligonucleotides grafted onto separate CNXL populations. The resulting hybrid nanomaterials were analyzed using dynamic light scattering, atomic force microscopy, and UV spectroscopy.