Poly(butylene
succinate) (PBS) is considered a promising biodegradable
material, whereas poor mechanical/thermal properties and low hydrolysis
rate restrict its further application. Herein, 1,4-butanediol (BDO)
was chemically grafted onto the graphene oxide (GO) surface by the
coupling effect of diisocyanate [e.g., 4,4′-diphenylmethane
diisocyanate (MDI), toluene diisocyanate (TDI), and hexamethylene
diisocyanate (HDI)], and the corresponding bionanocomposites were
prepared via in situ polymerization. By comparison, MDI has higher
reactivity with GO and BDO due to induction and the spatial steric
effect, and a strong interfacial covalent interaction of GO–MDI–PBS
was formed. Therefore, more PBS molecules were grafted onto GO and
intercalated into nanosheet layers to achieve a uniform dispersion
in the matrix. GO–MDI–PBS-0.5 wt % exhibited the maximum
tensile strength (39.96 MPa), elongation at break (458.48%), and notched
impact strength (9.80 kJ/m2), nearly 21.27, 44.58, and
127.91% increase than those of neat PBS, respectively, achieving simultaneous
improvement in mechanical strength and toughness. Besides, effective
intercalation enlarged the contact area with free radicals, resulting
in extraordinary radical scavenging ability of GO, and the excellent
oxygen barrier property of the composite was enhanced because the
uniform dispersion of GO sheets caused a more tortuous diffusion pathway
for oxygen, which endowed GO–MDI–PBS with remarkable
thermal–oxidative stability. Furthermore, GO–MDI–PBS
exhibited the improvement of crystallization rate, surface hydrophilicity,
and water vapor barrier properties, effectively promoting hydrolysis.