Abstract: Cellulose nanocrystals (CNC) possess high stiffness and thermostability that can become biomass-based composite materials/plastics for multipurpose use. In order to enhance the reusability, recyclability and reproducibility of CNC, polyurea with hindered urea bonds (HUB) was introduced to react with CNC. Upon reversible urea bonds formation, CNC can form carbamate bonds with polyurea to form new biomass-based plastics. Later, the residual diamine could form the polyurea with terephthalate and reproduce cellulose to complete the cycle. This crosslinked cellulose would feature high stiffness/thermostability from cellulose moieties, and reproducibility from polyurea with hindered urea bonds. This new cellulose-based material could be potentially applicable to various use such as construction materials and automotive materials in the future.