Covalently Functionalized Carbon Nano-Onions Integrated Gelatin Methacryloyl Nanocomposite Hydrogel Containing γ-Cyclodextrin as Drug Carrier for High-Performance pH-Triggered Drug Release

Herein, poly (n-(4-aminophenyl) methacrylamide)) carbon nano-onions (PAPMA-CNOs = f-CNOs) and γ-cyclodextrin/DOX-complex (CD) reinforced gelatin methacryloyl (GelMA)/f-CNOs/CD supramolecular hydrogel interfaces were fabricated using the photo-crosslinking technique. The physicochemical properties, morphology, biodegradation, and swelling properties of hydrogels were investigated. The composite hydrogels demonstrated enriched drug release under the acidic conditions (pH 4.5 = 99%, and pH 6.0 = 82%) over 18 days. Owing to the f-CNOs inclusion, GelMA/f-CNOs/CD supramolecular hydrogels presented augmented tensile strength (σ(ult) = 356.1 ± 3.4 MPa), toughness (K = 51.5 ± 0.24 Jg(−1)), and Young’s modulus (E = 41.8 ± 1.4 GPa). The strengthening of GelMA/f-CNOs/CD hydrogel systems indicates its good dispersion and the degree of polymer enveloping of f-CNOs within GelMA matrixes. Furthermore, the obtained hydrogels showed improved cell viability with human fibroblast cells. Nevertheless, the primed supramolecular hydrogels would pave the way for the controlled delivery systems for future drug delivery.