To
improve the mechanical properties of collagen hydrogels, which
are widely utilized as biomaterials, post-cross-linking of collagen
hydrogels was performed using polyrotaxane (PRX) as a cross-linker.
Herein, carboxymethyl group-modified PRXs (CMPRs) composed of carboxymethylated
α-cyclodextrins (α-CDs) threaded along poly(ethylene glycol)
(PEG) capped with bulky stoppers were used to cross-link via reaction
with the amino groups in the collagen. Four series of CMPRs with different
α-CD threading ratios and axle PEG molecular weights were used
for the post-cross-linking of the collagen hydrogels to verify the
optimal CMPR chemical compositions. The post-cross-linking of the
collagen hydrogels with CMPRs improved the swelling ratios and mechanical
properties, such as viscoelasticity and tensile strength. Among the
tested CMPRs, CMPRs with an axle PEG molecular weight of 35,000 (PEG35k)
resulted in better mechanical properties than CMPRs with a PEG10k
axis. Additionally, the cell adhesion and proliferation were greatly
improved on the surface of the collagen hydrogels post-cross-linked
with CMPRs with the PEG35k axle. These findings suggest that the molecular
weight of an axle polymer in CMPRs is a more important parameter than
the α-CD threading ratios. Accordingly, the post-cross-linking
of hydrogels with PRXs is promising for improving the mechanical properties
and biomaterial functions of collagen hydrogels.