▎ 摘　　要

Graphene-based magnetic materials exhibit novel properties and promising applications in the development of next-generation spintronic devices. Modern synthesis techniques have paved the way to design precisely the local environments of metal atoms anchored onto a nitrogen-doped graphene matrix. Herein, it is demonstrated that grafting cobalt (Co) into the graphene lattice induces robust and stable room-temperature ferromagnetism. These comprehensive experiments and first-principles calculations unambiguously identify that the mechanism for this unusual ferromagnetism is pi-d orbital hybridization between Co d(xz) and graphene p(z) orbitals. Here, it is found that the magnetic interactions of Co-carbon ions are mediated by the spin-polarized graphene p(z) orbitals, and room temperature ferromagnetism can be stabilized by electron doping. It is also found that the electronic structure near the Fermi level, which sets the nature of spin polarization of graphene p(z) bands, strongly depends on the local environment of the Co moiety. This is the crucial, previously missing, ingredient that enables control of the magnetism. Overall, these observations unambiguously reveal that engineering the atomic structure of metal-embedded graphene lattices through careful d to p orbital interactions opens a new window of opportunities for developing graphene-based spintronics devices.