Using
functionalized nanoparticles to crosslink hydrophilic polymers
is a growing theme of directly constructing nanocomposite (NC) hydrogels.
Employing dynamic covalent chemistry at the nanoparticle–polymer
interface is particularly attractive due to the spontaneous formation
and reversible manner of dynamic covalent bonds. However, the structure
and property modulation of the dynamic covalently crosslinked NC hydrogels
has not been thoroughly discussed. Here, we fabricated NC hydrogels
by using amine-functionalized carbon dots (CDs) to crosslink polydextran
aldehyde (PDA) polymers through imine bond formation. The role of
PDA with different oxidation degrees (i.e., PDA10, PDA30, and PDA50)
in affecting the microstructures and properties of PDA@CD hydrogels
was systematically investigated, showing that the PDA50@CD hydrogel
presented the densest structure and the highest mechanical strength
among the three PDA@CD hydrogels. The pH-responsiveness, 3D printing,
electrospinning, and biocompatibility of PDA@CD hydrogels were also
demonstrated, showing the great promise of using PDA@CD hydrogels
for applications in biomedicine and biofabrication.