Summary: In this report, we present a description of the optical and electronic properties of as-deposited, annealed, and chemically treated single-walled carbon nanotube (SWNT) films showing metallic or semiconducting behavior. As-deposited and annealed semiconducting SWNT films were significantly less conductive than metallic SWNT films; however, chemical treatment of semiconducting SWNT films resulted in sheet resistance values as low as 60 Ω·sq−1 in comparison to 76 Ω·sq−1 for similarly processed metallic SWNT films. We conclude that the greater improvement of electrical conductivity observed in the semiconducting SWNT film results from the difference in the density of available electronic states between metallic and semiconducting SWNTs. A corroborative investigation of the change in surface work function and the chemical composition of SWNT films, as revealed by X-ray photoelectron spectroscopy, is provided to support these conclusions and to give new perspective to the formation of electronically homogeneous SWNT networks.