The redox behavior of Sc3N@C-68 is studied systematically by means of electrochemistry, in situ ESR/Vis-NIR spectroelectrochemistry, and detailed theoretical treatment. Formation of the negatively and positively charged paramagnetic species for the same trimetallic nitride endohedral fullerene is demonstrated for the first time. The electrochemical study of Sc3N@C-68 exhibits two electrochemically irreversible but chemically reversible reduction steps and two reversible oxidation steps. A double-square reaction scheme is proposed to explain the observed redox reaction at cathodic potentials involving the reversible dimerisation of the Sc3N@C-68 monoanion. The spin state of the radical cation and the radical anion is probed by ESR spectroscopy, indicating that in both states, the large part of the unpaired spin is delocalized on the fullerene cage. The charged states of the non-isolated pentagon rule fullerene are characterized furthermore by in situ absorption spectroscopy. The interpretation of experimental data is supported by the density functional theory (DFT) calculations of the spin distribution in the anion and cation radicals of Sc3N@C-68 and time-dependent DFT calculations of the absorption spectra of the charged species.