In this investigation, the preparation of novel Halloysite-based chitosan/oxidized starch (Hal/CTS/OSR) Hybrid bionanocomposite hydrogels is described. The obtained hybrid hydrogels were characterized by using FT-IR, SEM, XRD, TGA and DTG techniques. In addition, the efficiency of hydrogels as drug delivery systems was studied. The results demonstrated that depending on experimental parameters, such as the ratio of CTS/OSR, and the type of Hal nanotubes (modified or unmodified), the hydrogel properties can be affected and modulated significantly. 74.3%, 71.2% and 69.45% MTZ release were observed for CTS/OSR/mHal 10, CTS/OSR and CTS/OSR/Hal 10 respectively.