Montmorillonite (MMt) is extensively applied as an efcient drug-carrier in designing drug delivery systems (DDS) due to its high specifc surface area to load drugs. Modifcation of MMt via iron (Fe) blending can thus be a desirable method to improve its biocompatibility. Herein, magnetic nano-carriers involving the magnetic MMt (mMMt) core surrounded by chitosan (Chito) as a biopolymer and hyaluronic acid (HA) were prepared. To coat the mMMt fabricated through the coprecipitation of the Fe3+/Fe2+ ions in the presence of MMt, the acquired mMMt as the core was then treated with the Chito/HA solution to induce the cross-linked Chito/HA as the shell (namely, the Chito/HA-mMMt). The transmission electron microscopy (TEM) results accordingly revealed the existence of the mMMt inside the Chito/ HA solution. Curcumin (CUR) and ciprofoxacin (CIP) were further employed as two model drugs. The CUR and CIP release from the Chito/HA-mMMt subsequently occurred in a sustained manner and pH-dependently. Additionally, an upsurge in the CUR and CIP release by applying an external magnetic feld was observed. Thus, the prepared Chito/HA-mMMt hydrogels promise an outstanding potential performance in terms of expanding novel pH-dependent DDS with a sustained release behavior. The scratch assay of the given hydrogels also confrms their applications for wound healing.