Data for characterization of S-enantiomer (levetiracetam) and racemic compound (etiracetam) of 2-(2-Oxo-1-pyrrolidinyl) butyramide by increasing pressure. The data was collected through single-crystal X-ray diffraction and Raman Spectroscopy. The single-crystal X-ray diffraction images are in the format .sfrm (Bruker program) and can be read in APEX software. The PIXEL data has been generated using Gaussian software (.gjf files) and PIXEL (.mlc, .pri files); the latter can be viewed in a text editor. The Raman spectroscopy data are in the .l6S format (LabSpec 6 program) and also .txt format that can be viewed using any data analysis software. The modification of single-crystal X-ray file names from the original names to those represented in the article is explained in .xlsx files visible in the main folder. The naming used in the PIXEL calculation follows those represented in the article.