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A nonlithographic patterning technique based on a numerically controlled atmospheric-pressure microplasma source has been developed to fabricate surface-enhanced Raman scattering (SERS) substrates. Microstructures in silver (Ag) films on glass are created by localized physical sputtering of Ag atoms using an argon (Ar) microplasma horizontally scanned across the glass substrate. Detection of crystal violet on patterned substrates shows an enhancement of the Raman scattering signal intensity by eight to ten orders of magnitude higher than bare Ag/glass substrates. The SERS enhancement depends on the pattern geometry showing that the mechanism is related to surface irregularities in the sputtered holes.