To further improve the efficiencies of the established drugs, various treatment strategies, such as preparation of protein-drug conjugates and the design of nanoscale drug-carriers, are used to increase the efficacy of therapeutic agents. [6-8] Several effective nanocarrier systems were designed to deliver anti-cancer cytotoxic agents to tumor cells with high selectivity and efficacy while minimizing negative side effects. [9,10] Drug nano-carriers provide multiple advantages, such as convenient uptake and internalization, reduced drug interactions, optimized lifetime, and widened therapeutic windows. [11] In this regard, the synthetic design and applications of different types of iron oxide nanoparticles (Fe 3 O 4 NPs) have received significant attention since these NPs can be magnetically directed inside target tissues and their surface can be easily functionalized with diverse polymers and organic compounds. [12-16] Previously, we have reported several magnetic systems in micro-and nanoscale for diverse functional applications. [17-24] To further expand upon this work, we utilized one of the most commonly employed polymers, polyvinyl alcohol (PVA), to encapsulate magnetic Fe 3 O 4 NPs by virtue of its extended hydrogen bonding and to provide a selective release medium for DXL. [25] Drug molecules, such as DXL, can be incorporated into a PVA gel when polymer chains are in a shrunk state at low temperatures, and subsequently released in a target tissue upon a PVA transition into a swollen gel at 37 °C. [26] PVA features several important advantages. First is the ability to form a gel owing to multiple hydrogen bonding by OH groups. A versatile breast cancer-targeting nanocomposite therapeutic combining docetaxel (DXL), polyvinyl alcohol (PVA) network for controlled release, and silica-protected magnetic iron oxide nanoparticles (Fe 3 O 4 NPs) for targeted delivery and gold nanoparticles (AuNPs) for plasmonic photothermal therapy (PPTT) is presented in this work. First, the designed nanocomposite is magnetically directed for cancer-targeted therapy confirmed by computerized tomography (CT) scans. Second, 10% DXL by mass is loaded into PVA, a pH and temperature responsive gel, for controlled release. Third, PPTT is confirmed with Au/Fe 3 O 4 /PVA-10%DXL using a prototype circulation system and then for tumor treatment in vivo; Au/Fe 3 O 4 /PVA-10%DXL is conveniently directed and the entrapped DXL is selectively released (≈96%) via the interaction of green and near-infrared (NIR) light with the localized surface plasmon resonance of AuNPs. A 75% cell death is reported from in vitro studies with DXL doses as low as 20 µg mL −1 of Au/Fe 3 O 4 /PVA-10%DXL, and a 70% tumor growth inhibition is demonstrated by in vivo experiments with the biosafety studies confirming minimal side effects to other organs. Overall, the developed Au/Fe 3 O 4 /PVA-10%DXL has a strong potential to simultaneously enhance CT imaging contrast together with the targeted delivery of DXL.