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Sample-preparation methods have been developed and adapted for using gold nanoparticles in qualitative analysis of paint layer compositions with surface-enhanced Raman scattering (SERS). Use of plasmonic nanoparticles for SERS analysis of art materials in actual paintings could significantly reduce the luminescent background caused by the presence of organic binders in the paint layer and led to multiple amplification of the chromophore Raman-line intensities and an increase in the signal-to-noise ratio. The techniques were successfully tested on paint layers of 12 easel paintings of the XVI–XIX centuries in close cooperation with museums of the Republic of Belarus and could be systematically used in art history expertise to identify the composition of paints and attribution of cultural heritage objects. [ABSTRACT FROM AUTHOR]