Fullerenes have several advantages as potential materials for organic spintronics.Through a theoretical first-principles study,we report that fullerene C60 adsorption can induce a magnetic reconstruction in a Ni(111)surface and expose the merits of the reconstructed C60/Ni(111) spinterface for molecular spintronics applications.Surface reconstruction drastically modifies the magnetic properties at both sides of the C60/Ni interface.Three outstanding properties of the reconstructed structure are revealed,which originate from reconstruction enhanced spin-split π-d coupling between C60 and Ni(111):(1)the C60 spin polarization and conductance around the Fermi level are enhanced simultaneously,which can be important for read-head sensor miniaturization;(2) localized spinpolarized states appear in C60 with a spin-filter functionality; and(3) magnetocrystalline anisotropic energy and exchange coupling in the outermost Ni layer are reduced enormously.Surface reconstruction can be realized simply by controlling the annealing temperature in experiments.