We deploy topographical and spectroscopic techniques to show that a strongly spin-polarized interface arises between ferromagnetic cobalt and an amorphous carbon layer. Scanning tunneling microscopy and spectroscopy show how a semiconducting carbon film with a low band gap of about 0.4 eV is formed atop the metallic interface. To understand how the cobalt/carbon interface is formed, we used X-ray photoemission spectroscopy to study the hybridization state of carbon. We find that the semiconducting layer consists mainly of sp²-bonded carbon atoms with a sp²-to-sp³ ratio between 1.4 and 1.8. The spin-polarized properties of the cobalt/carbon interface are studied by spin-resolved photoemission spectroscopy. We observe interface states close to the Fermi energy that are not exclusive to cobalt. These electronic states reveal a high degree of spin polarization at room temperature. (C) 2015 Elsevier Ltd. All rights reserved.