Paramagnetic endohedral fullerenes are ideal candidates for quantum information processing and high-density data storage due to their protected spins with particularly high stability. Herein, we report a solid spin system based on a paramagnetic metallofullerene Y-2@e(79)N through incarcerating it into the cage-shaped pores of a metal organic framework (MOF-177). In this kind of guest and host complex, the Y-2@C79N molecules inside the pores of MOP crystal show axisymmetric paramagnetic property. It was found that the pores of MOF-177 crystal play an important role in dispersing the Y-2@e(79)N molecules as well as in steering their electron spin. The group of arranged Y-2@e(79)N molecules and their electron spins in MOF crystals are potential quantum bits for quantum information science and data storage. Moreover, this kind of solid spin system can be used as a probe for nanoscale nuclear magnetic resonance or for motion imaging of a single biomolecule.