Chondroitin
sulfate (CS), the main component of cartilage extracellular
matrix, has attracted attention as a biomaterial for cartilage tissue
engineering. However, current CS hydrogel systems still have limitations
for application in successful cartilage tissue engineering owing to
their unsuitable degradation kinetics, insufficient mechanical similarity,
and lack of integration with the native cartilage tissue. In this
study, using mussel adhesive-inspired catechol chemistry, we developed
a functional CS hydrogel that exhibits tunable physical and mechanical
properties as well as excellent tissue adhesion for efficient integration
with native tissues. Various properties of the developed catechol-functionalized
CS (CS-CA) hydrogel, including swelling, degradation, mechanical properties,
and adhesiveness, could be tailored by varying the conjugation ratio
of the catechol group to the CS backbone and the concentration of
the CS-CA conjugates. CS-CA hydrogels exhibited significantly increased
modulus (∼10 kPa) and superior adhesive properties (∼3
N) over conventional CS hydrogels (∼hundreds Pa and ∼0.05
N). In addition, CS-CA hydrogels incorporating decellularized cartilage
tissue dice promoted the chondrogenic differentiation of human adipose-derived
mesenchymal stem cells by providing a cartilage-like microenvironment.
Finally, the transplantation of autologous cartilage dice using tissue-adhesive
CS-CA hydrogels enhanced cartilage integration with host tissue and
neo-cartilage formation owing to favorable physical, mechanical, and
biological properties for cartilage formation. In conclusion, our
study demonstrated the potential utility of the CS-CA hydrogel system
in cartilage tissue reconstruction.