A study to observe higher vibrational levels in NCO((A) over tilde (2) Sigma(+)) and the onset of predissociation in this molecule has been carried out. Laser fluorescence spectra have been recorded over the wave number range 27 300-32 900 cm(-1), from the (A) over tilde(0,0,2)-(X) over tilde(0,0,0) band up through the (B) over tilde(1,0,0)-(X) over tilde(0,0,0) band. Vibrational assignments have been made for a number of newly observed (A) over tilde-(X) over tilde bands, and band origin wave numbers and upper level rotational constants have been derived from comparison of experimental spectra with simulations. Decay lifetimes for excitation of a large number of both assigned and unassigned excited vibronic levels have been determined. The onset of predissociation appears to occur at energies slightly below that of the (B) over tilde(0,0,0) level.