The jet-cooled FTIR spectrum of the nu (6) fundamental band (C-O stretch) of vanadium hexacarbonyl, V(CO)(6), is studied for the first time. The spectrum shows a very unusual structure consisting of three well-defined broad subbands, without the usual PQR structure. V(CO)(6) being an open-shell system this is attributed to a dynamical F-2g x F-1u Jahn-Teller coupling which considerably complicates the analysis. A new theoretical model based on group theory and tensorial algebraic techniques is developed in this paper for the very first attempt to analyze such a rovibronic spectrum. The assumption of a negligible spin-orbit coupling is validated by the overall agreement between predicted and observed band profiles. The rovibronic Hamiltonian and dipole moment operators have been expanded in order to enable a simultaneous treatment of the four vibronic sublevels. We were able to satisfactorily reproduce the band profile and thus to give the first estimation of some rovibronic parameters for this molecule.