Regulation of cell‐substrate interactions is an important factor for modulating cell behaviors. Tailoring the physical and chemical properties of the substrates to better mimic the extracellular matrix (ECM) of native tissue is a more effective strategy for enhancing the cell‐substrate contact. In current work, we aim at improving surface bioactivity based on the liquid crystalline substrates for the enhancement in cell affinity and osteogenic differentiation. Polydopamine (PDOPA) adhesive coating was used as a reactive platform for the immobilization of chitooligosaccharide (COS) on the octyl hydroxypropyl cellulose ester (OPC) substrate to generate active OPC‐PDOPA‐COSs liquid crystalline substrates. Results demonstrated that PDOPA‐coated OPC surfaces showed remarkably improved hydrophility and increased elastic modulus, leading to better initial cell attachment. Subsequent COS immobilization on the OPC‐PDOPA layer could induce promotion of cell proliferation, polarization and cytoskeleton formation. Rat bone marrow mesenchymal stem cells (rBMSCs) seeded on the OPC‐PDOPA‐COSs showed higher alkaline phosphatase (ALP) activity, calcium deposition, and up‐regulated bone‐related genes expression, including BMP‐2, RUNx‐2, COL‐I and OCN. In conclusion, surface biofunctionalization on the OPC‐based liquid crystalline substrates could come into being the appropriate combination of surface chemistry and liquid crystalline characteristic that simulating in vivo ECM environment, resulting in a favorable support to enhance positive cell‐substrate interactions.

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