The quality of surface coating of magnetic nanoparticles destined as nanoprobes in clinical applications is of utmost significance for their colloidal stability and biocompatibility. A novel approach for the fabrication of such a coating involves the synthesis of well-defined diblock copolymers based on 2-(acetoacetoxy)ethyl methacrylate (chelating) and poly(ethylene glycol)methyl ether methacrylate (water-soluble, thermoresponsive), prepared by reversible addition-fragmentation chain transfer polymerization. Fabrication of magneto-responsive micelles was accomplished via chemical coprecipitation of Fe(III)/Fe(II) in the presence of diblock copolymers. Further to the characterization of micellar morphologies, optical and thermal properties, assessment of magnetic characteristics disclosed superparamagnetic behavior. The hybrid micelles did not compromise cell viability in cultures, while in vitro uptake by macrophage cells was significantly lower in comparison to that of the clinically applicable contrast agent Resovist, suggesting that these systems can evade rapid uptake by the reticuloendothelial system and be useful agents for in vivo applications.