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We report on the use of an atmospheric pressure, open-air plasma treatment to remove Li2CO3 species from the surface of garnet-type tantalum-doped lithium lanthanum zirconium oxide (Li6.4La3Zr1.4Ta0.6O12, LLZTO) solid-state electrolyte pellets. The Li2CO3 layer, which we show forms on the surface of garnets within 3 min of exposure to ambient moisture and CO2, increases the interface (surface) resistance of LLZTO. The plasma treatment is carried out entirely in ambient and is enabled by use of a custom-built metal shroud that is placed around the plasma nozzle to prevent moisture and CO2 from reacting with the sample. After the plasma treatment, N2 compressed gas is flowed through the shroud to cool the sample and prevent atmospheric species from reacting with the LLZTO. We demonstrate that this approach is effective for removing the Li2CO3 from the surface of LLZTO. The surface chemistry is characterized with X-ray photoelectron spectroscopy to evaluate the effect of process parameters (plasma exposure time and shroud gas chemistry) on removal of the surface species. We also show that the open-air plasma treatment can significantly reduce the interface resistance. This platform demonstrates a path towards open-air processed solid-state batteries.