The spectrum of the Fe I atom is critical to many areas of astrophysics and beyond. Measurements of the energies of its high-lying levels remain seriously incomplete. Here we update the work by Peterson & Kurucz (2015) to identify such levels using new and archival high-resolution absorption-line UV and optical spectra of stars whose warm temperatures favor Fe I lines. Our GO-14161 Hubble program will obtain UV spectra for four metal-poor turnoff stars, archive them at ASTRAL, and draw from them the new identifications of 250 – 500 Fe I levels.