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Nanoparticulate agents for magnetic drug delivery systems (DDSs) have extensive applications in targeted drug delivery, contrast imaging and therapeutics. However, no simple synthetic method for magnetic DDS agents has been developed without the need to add magnetic nanoparticles. Here, we describe the one-step fabrication of ‘all-in-one’ magneto-assemblies using an ‘inorganic-metal-salt-free’ method, involving spontaneous self-assembly of the water-insoluble prodrug μ-oxo-bis(N,N′-ethylenebis(salicylideniminato)iron) [Fe(salen)] (magnetic core) with polypyrrole (PPy)-b-polycaprolactone (PCL) smart diblock copolymers. In the system, PCL serves as a heat-responsive core scaffold, and PPy serves as an electronic core-size controller and pH-responsive shell. This core–shell nanocomposite has a high-loading capacity (~90%), and the core size is tunable by incorporating albumin or gum arabic as bio-coating agents, which also provide colloidal stability, biocompatibility and thermo-stability. Fe(salen), which has intrinsic antitumor activity, also has ubiquitous magnetic properties, which are dramatically enhanced in these molecular assemblies with magnetic coupling. Moreover, these multifunctional nanoassemblies can be delivered magnetically, can serve as magnetic resonance imaging contrast agents, can generate magneto-hyperthermal effects and can enable magnetic field-triggered release of Fe(salen) molecules under acidic conditions.

Magnetic metal-complex-conducting copolymer core–shell nanoassemblies for a single-drug anticancer platform