The Fe I spectrum is critical to many areas of astrophysics, yet many of the high-lying levels remain uncharacterized. To remedy this deficiency, Peterson & Kurucz (2015, J/ApJS/216/1) identified Fe I lines in archival ultraviolet and optical spectra of metal-poor stars, whose warm temperatures favor moderate Fe I excitation. Sixty-five new levels were recovered, with 1500 detectable lines, including several bound levels in the ionization continuum of Fe I. Here, we extend the previous work by identifying 59 additional levels, with 1400 detectable lines, by incorporating new high-resolution UV spectra of warm metal-poor stars recently obtained by the Hubble Space Telescope Imaging Spectrograph. We provide gf values for these transitions, both computed as well as adjusted to fit the stellar spectra. We also expand our spectral calculations to the infrared, confirming three levels by matching high-quality spectra of the Sun and two cool stars in the H-band. The predicted gf values suggest that an additional 3700 Fe I lines should be detectable in existing solar infrared spectra. Extending the empirical line identification work to the infrared would help confirm additional Fe I levels, as would new high-resolution UV spectra of metal-poor turnoff stars below 1900{AA}.