On the summit of Kilauea volcano, sulfur dioxide, which is continuously emitted from Halemaumau crater and rapidly sequestered into sulfuric-acid–rich aerosol entrained in the prevailing trade winds, is subsequently precipitated as acid fog immediately downwind from Kilauea caldera in the Kau Desert. The characteristic pH of surface tephra deposits is <4.0 in Sand Wash, a region of nearly continuous, acidic aerosol fallout immediately southwest of the caldera. Vertical exposures of unconsolidated tephras of the Keanakakoi Ash found within fissures and small, dry gullies are coated with thin rock coatings of amorphous silica and jarosite. These rock coatings are formed via an evaporative mechanism whereby acidic pore fluids, circulating in the upper few meters within the highly porous tephra, are wicked toward the walls of the gullies. Geochemical modeling of the rock coating formation process implies that the sulfate formation via evaporation occurs subsequent to minimal interaction of acidic pore fluids with the basaltic tephra. This also suggests that the cycle from acid-fog fallout to precipitation of the siliceous-sulfate rock coatings must occur quite rapidly. Acid-fog deposition of sulfate and silica at Kilauea may provide one mechanism for the origin of jarosite-bearing outcrops on Mars.