New information on the experimentally determined vibrational and electronic energy levels of approximately 500 neutral and ionic transient molecules possessing from 3 to 16 atoms has been evaluated and added to the previously established database for these species. There has been selective extension of the compilation to somewhat less reactive species such as HNCO, HCNO, H2O2, and cis- and trans-HONO, as well as to many transient molecules which include atoms beyond the third row of the Periodic Table. Electronic spectral data are also given for a number of transient molecules which possess more than six atoms. Radiative lifetimes and the principal rotational constants are included. Observations in the gas phase, in molecular beams, and in rare-gas and nitrogen matrices are evaluated. The types of measurement surveyed include conventional and laser-based absorption and emission techniques, laser absorption with mass analysis, and photoelectron spectroscopy.