Ab initio calculations have been carried out on the 1,3,5,7- and 1,2,4,7-tetraene configurations of the cyclooctatetraenyl radical at UHF, ROHF, MCSCF, ROCISD, QCISD, and CCSD(T) levels of theory with 6-311G(d,p) and cc-pVDZ basis sets. Although spin contamination is present, the ROCISD calculations support the energies obtained from less intensive, UHF-based coupled cluster calculations over the energies obtained from MCSCF analysis of the pi-electron orbitals. The 1,3,5,7-form is a local minimum at the coupled cluster levels, higher in energy than the resonance-stabilized 1,2,4,7-form by 10-13 kJ/mol, but bounded by a barrier of less than 0.5 kJ/mol. The isomerization surface connecting these two structures is described and results reported from integration of the vibrational Schrödinger equation on that surface. Excited vibrational states at energies just above the isomerization barrier are dominated by the character of the 1,3,5,7-tetraenyl radical, which suggests that chemistry involving this intermediate at typical combustion temperatures may branch at this juncture.