Magnetic core–polymer shell nanoparticles, with the core mainly in the form of magnetite (Fe
3
O
4
) or maghemite (γ‐Fe
2
O
3
), offer great opportunities for applications in biomedicine. Such a configuration provides a synergistic combination of the intrinsic properties of the magnetic core with special biochemical functions, achieved through proper tailoring of the polymer shell. Active research and development efforts on the applications of such nanoparticles are ongoing in biomedical areas, such as contrast agents for magnetic resonance imaging to achieve increasingly high spatial resolution, down to the cellular and even molecular level; delivery vehicles of drugs to targeted organs or tumors; and as a heating mediator for cancer thermotherapy (hyperthermia). The controllability of these nanoparticles with respect to their physico‐chemical properties, biodistribution and site specificity within the physiological environment, are major challenges which need to be addressed. In this chapter we review the synthetic routes of magnetic core–polymer shell nanoparticles, with emphasis on the tailoring of the polymer shell to confer the nanoparticles with desired properties for biomedical applications.