The understanding of orbital hybridization and spin polarization at the organic-ferromagnetic interface is essential in the search for efficient hybrid spintronic devices. Here, using first-principles calculations, we report a systematic study of spin-split hybrid states of C60 deposited on various ferromagnetic surfaces: bcc-Cr(001), bcc-Fe(001), bcc-Co(001), fcc-Co(001), and hcp-Co(0001). We show that the adsorption geometry of the molecule with respect to the surface crystallographic orientation of the magnetic substrate as well as the strength of the interaction play a crucial role in the spin polarization of the hybrid orbitals. We find that a large spin polarization in vacuum above the buckyball can only be achieved if the molecule is adsorbed upon a bcc-(001) surface by its pentagonal ring. Therefore, bcc-Cr(001), bcc-Fe(001), and bcc-Co(001) are the optimal candidates. Spin-polarized scanning tunneling spectroscopy measurements on single C60 adsorbed on Cr(001) and Co/Pt(111) also confirm that the symmetry both of the substrate and of the molecular conformation has a strong influence on the induced spin polarization. Our finding may give valuable insights for further engineering of spin filtering devices through single molecular orbitals.