Bio-based epoxy resins are being used due to their green chemistry. They have better properties than petroleum-based epoxy resins. Recently, environment friendly nanomaterials have been used for different industrial applications. Cellulose nanocrystals (CNCs) are among the best naturally occurring materials.Therefore, the surface of cellulose nanocrystals are modi ed by eugenol-based silane coupling agent (EBSCA). Chemical composition and surface morphologies of CNCs were analyzed and characterized by FTIR, AFM, SEM, TEM and 1 H-NMR. The SEM and AFM results con rmed eugenol-based silane coupling agent was successfully grafted on cellulose nanocrystals. Modi ed CNCs demonstrated an excellent tensile strength (2190 MPa) and modulus (16.00 MPa), as well as storage modulus (1622 MPa) exhibited by 1wt% modi ed cellulose nanocrystals composites. Additionally, modi ed CNCs displayed hydrophobic behavior (CA=102 ± 2°). The corresponding modi ed CNCs have signi cant applications in combination of high stiffness and strength to the epoxy resins. This study lays a foundation towards full bio-based, environment friendly polymers fabrication and consumptions most desirable in adhesive and mechanical industrial elds.