The aim of the present work was to develop green carriers for methotrexate using -carrageenan/chitosan complexes. Magnetic Fe3O4 nanoparticles were first synthesized in the presence of -carrageenan through in situ method. Then, the obtained magnetic -carrageenan was crosslinked using the polycation chitosan biopolymer. The physical and structural properties of hydrogels were investigated by FTIR, XRD, SEM, TEM, TGA, and VSM techniques. The pH-dependent swelling behavior of hydrogels was examined in various buffer solutions. All of the prepared hydrogels showed a high swelling capacity in basic solutions. The introduction of magnetite nanoparticles into -carrageenan/chitosan complexes had a significant effect on the swelling capacity of magnetic hydrogels, as the water absorbency of hydrogels decreased with increasing magnetite content. Methotrexate as an anticancer and model drug was loaded on hydrogels and the release profiles were investigated at pH = 7.4 and 5.3. The methotrexate encapsulation efficiency was increased by increasing magnetite and chitosan contents. The results demonstrated that the release of methotrexate from magnetic hydrogels is pH-dependent with a high release content at pH = 7.4. The release profiles were analyzed by Peppas’s empirical model and the release of drug from hydrogels followed Fickian type of diffusion mechanism at both pHs.
