. The Fe/FeCaP particles annealed at 600 °C show a much higher magnetic moment compared with the non-annealed FeCaP particles. Moreover, T2-weighted MRI phantom images reveal that the Fe/FeCaP heterostructured microspheres possess higher relaxivity than paramagnetic FeCaP, demonstrating their potential as superior and biocompatible MRI contrast agents. Moreover, the enhancement in osteoconductivity for Fe/FeCaP microspheres without any evidence of cytotoxicity was verified. Our results demonstrate the great potential of multi-functional Fe/FeCaP microspheres for use as biocompatible bone regeneration agents as well as MRI contrast agents.