We have prepared a magnetite encapsulated polymer nanocomposite (MEPN) by an emulsification-diffusion technique and found that the encapsulation efficiency could be precisely controlled according to the portion of magnetite and the capping ligand that covers the surface of the magnetite nanoparticles. The field-dependence and temperature dependence on magnetization, measured by a superconducting quantum interference device, demonstrate that there was no size effect of the magnetite nanoparticles on the encapsulation behavior. The size distribution and T2 relaxivity of prepared MEPNs were measured using magnetic resonance imaging for analysis of the effect of aggregation and it was verified that aggregates of the magnetite nanoparticles provide enhanced relaxation ability.