Montmorillonite (MMt) is a widely utilized material in the development of wound dressing patches because of its large specific surface area, which allows for efficient drug loading. Blending iron (Fe) with MMt can be a beneficial approach to enhance its biocompatibility. Herein, the prepared magnetic MMt nanoparticles (mMMt NPs) were grafted into chitosan (Chito), hyaluronic acid (HA), and polyvinyl alcohol (PVA) as a nanofiber (Chito/HA/PVA-mMMt nanofiber). The results displayed that the mMMt NPs were distributed in the Chito/HA/ PVA nanofiber mat. The utilization of curcumin (CUR) as a model drug was subsequently employed. The release of CUR from the magnetic nanofibers then happened consistently and continuously, dependent on the pH. Furthermore, an increase in CUR release was observed when a magnetic field from an external source was applied. Therefore, the synthesized Chito/HA/PVA-mMMt nanofibers show great potential for use in the development of innovative wound dressing patches with pH-dependent behavior and sustained release. These nanofibers can be applied in transdermal drug delivery systems and wound healing approaches, offering promising performance.