This work aimed to design montmorillonite-incorporated pH-responsive and magnetic κ-carrageenan/chitosan hydrogels via a completely green route for controlled release of sunitinib anticancer drug. This was accomplished by ionic cross-linking of two biopolymers, κ-carrageenan and chitosan, in the presence of magnetic montmorillonite (mMMt) nanoplatelets. Interestingly, it was observed that the amount of mMMt affected not only the microstructure of hydrogels, but also the drug loading efficiency of nanocomposite hydrogels was noticeably increased by introducing mMMt (from 69 to 96%). The in vitro sunitinib release experiments showed that a low content of loaded sunitinib was released from all hydrogels in the buffered solution with pH 7.4. In contrast, a relatively sustained release with a high content of drug release was observed in the acidic solution of pH 5.5. During 48 h, the hydrogels nanocomposite containing a high content of mMMt showed cumulative release of 64.0 and 8.6% at pH 5.5 and 7.4, respectively. During two days, while the cumulative release of sunitinib was obtained 84.3% for the magnetic-free hydrogel, the magnetic ones showed 74.4 and 64% with the low and high contents of magnetic MMt, respectively. The developed κ-carrageenan/chitosan hydrogels with a high capacity of drug loading and subsequent pH-sensitive drug release can be considered in prolonged cancer therapy with reduced side effects.
