A series of biodegradable poly (butylene succinate-co-terephthalate) (PBST) with different aromatic units content was synthesized and then melt blended by adding cellulose nanocrystals (CNCs) to manufacture the full organic composites. A network-like structure of CNCs in PBST matrix was evaluated by rheometer. The storage modulus and complex viscosity at low frequency region were significantly enhanced with increasing CNC content. Meanwhile, the decreasing tan delta and flow index were attributed to the excellent interaction between PBST and CNCs. When PBST has a content of the aromatic unit exceeds 30 mol%, the crystallization temperatures increased with increasing CNC contents. On the other hand, when PBST has 30 mol% content of the aromatic unit, the cold crystallization temperatures decreased with increasing CNC contents. These above observation in crystallization properties suggested that the CNC make a role of heterogeneous nucleation in PBST matrix. The result of mechanical properties evaluated by dynamic mechanical analysis showed a good reinforcement effect of the addition of stiff CNC. The PBST/CNC composites were suitable for cell growth and might have a potential as biomedical materials, which is confirmed by MTT assay.