The
osteochondral lesions and osteoarthritis-related complications
continue to be clinically relevant challenges to be addressed by the
biomaterials community. Hydrogel-based scaffolds have been widely
investigated to enhance osteochondral regeneration, but the inferior
mechanical properties together with poor functional stability are
the major constraints in their clinical translation. The development
of osteochondral implants with natural tissue-mimicking mechanical
properties remains largely unexplored. In this perspective, the present
study demonstrates a strategy to develop a bilayer osteochondral implant
with an elastically stiff composite (poly(vinylidene difluoride)-reinforced
BaTiO3, PVDF/BT) and elastically compliant composite (maleic
anhydride-functionalized PVDF/thermoplastic polyurethane/BaTiO3, m-PVDF/TPU/BT). The compositional variation in polymer composites
allowed the elastic modulus of the hybrid bilayer construct to vary
from ∼2 GPa to ∼90 MPa, which enabled a better understanding
of the substrate-stiffness-dependent cellular behavior and maturation
of preosteoblasts and chondrocytes. The cellular functionalities on
PVDF-based polymer matrices have been benchmarked against ultrahigh-molecular-weight
polyethylene (UHMWPE), which is clinically used for a wide spectrum
of orthopedic applications. The increased alkaline phosphatase (ALP)
activity, collagen synthesis, and matrix mineralization confirmed
the early differentiation of preosteoblasts on the PVDF/BT matrix
with subchondral bone-like mechanical properties. On the contrary,
the upregulated chondrogenic functionalities were recorded on m-PVDF/TPU/BT
with an elevated level of collagen content, glycosaminoglycans, and
proteoglycans. Emphasis has been laid on probing the regulation of
the osteochondral behavior using tailored substrate stiffness and
functionalities using compatibilized fluoropolymer-based elastomeric
composites. Taken together, the results of this work conclusively
establish the efficacy of the hybrid bilayer composite with natural
tissue-mimicking mechanical properties for the functional repair of
osteochondral defects.