This paper summarizes the Spirit rover operations in the Columbia Hills of Gusev Crater from sols 513 to 1476 and provides an overview of selected findings that focus on synergistic use of the Athena Payload and comparisons to orbital data. Results include discovery of outcrops (Voltaire) on Husband Hill that are interpreted to be altered impact melt deposits that incorporated local materials during emplacement. Evidence for extensive volcanic activity and aqueous alteration in the Inner Basin is also detailed, including discovery and characterization of accretionary lapilli and formation of sulfate, silica, and hematite‐rich deposits. Use of Spirit's data to understand the range of spectral signatures observed over the Columbia Hills by the Mars Reconnaissance Orbiter's Compact Reconnaissance Imaging Spectrometer (CRISM) hyperspectral imager (0.4–4 μm) is summarized. We show that CRISM spectra are controlled by the proportion of ferric‐rich dust to ferrous‐bearing igneous minerals exposed in ripples and other wind‐blown deposits. The evidence for aqueous alteration derived from Spirit's data is associated with outcrops that are too small to be detected from orbital observations or with materials exposed from the shallow subsurface during rover activities. Although orbital observations show many other locations on Mars with evidence for minerals formed or altered in an aqueous environment, Spirit's data imply that the older crust of Mars has been altered even more extensively than evident from orbital data. This result greatly increases the potential that the surface or shallow subsurface was once a habitable regime.