Previous experimental assignments of the fundamental vibrational frequencies of NCCO have been brought into question by subsequent unsuccessful attempts to observe IR signatures of this radical at these frequencies. Here we compute the fundamental vibrational frequencies by applying second-order vibrational perturbation theory to the complete quartic force field computed at the all-electron (AE) coupled cluster singles, doubles, and perturbative triples level [CCSD(T)] with the correlation-consistent, polarized core-valence quadruple-zeta (cc-pCVQZ) basis set, which has tight functions to correctly describe core correlation. The AE-CCSD(T)/cc-pCVQZ geometric parameters are r(e)(N-C)=1.1623 A, r(e)(C-C)=1.4370 A, r(e)(C-O)=1.1758 A, theta(e)(N-C-C)=168.55 degrees , and theta(e)(C-C-O)=132.22 degrees . Our CCSD(T)/cc-pCVQZ values of the characteristic stretching frequencies nu(1) and nu(2) are 2171 and 1898 cm(-1), respectively, in stark contrast to the experimentally derived values of 2093 and 1774 cm(-1). Finally, focal-point extrapolations using correlation-consistent basis sets cc-pVXZ (X=D,T,Q,5,6) and electron correlation treatments as extensive as full coupled cluster singles, doubles, and triples (CCSDT) with perturbative accounting of quadruple excitations [CCSDT(Q)] determine the vibrationless barrier to linearity of NCCO and the dissociation energy (D(0)) of NCCO-->NC+CO to be 8.4 and 26.5 kcal mol(-1), respectively. Using our precisely determined dissociation energy, we recommend a new 0 K enthalpy of formation for NCCO of 50.9+/-0.3 kcal mol(-1).