The unique structure of endohedral metallofullerenes leads to well protected internal species by the fullerene cages, so even those highly reactive radicals such as N, Sc3C2 etc. can be stabilized to form stable paramagnetic molecules (e.g. N@C60, Sc3C2@C80). However, a challenge is how to manipulate the magnetic property of the internal species from outside of the fullerene cages. Herein we reported a technique to achieve a well manipulation of the electronic spin of a paramagnetic endohedral fullerene Sc3C2@C80 by connecting it with nitroxide radical to form a two spin center molecule FSc3C2@C80PNO·. Based on the adjustable spin-spin interactions between Sc3C2@C80 and NO· groups, the magnetic property of Sc3C2@C80 is indirectly controlled by the NO· group.