This dataset contains descriptions and analytical data (i.e., electron microprobe, X-ray diffraction, spectral reflectance, and scanning electron microprobe analyses) for unexpanded and expanded vermiculite samples. These data are provided for 52 samples of vermiculite attic insulation, horticultural products, aggregate, and packing materials derived from mines near Enoree, South Carolina; Libby, Montana; Louisa, Virginia; Palabora, South Africa; and Jiangsu, China collected from 2000 to 2016. Electron probe microanalysis and spectra of unexpanded ores from these locations and Llano, Texas are also given. Tables of electron microprobe and spectral absorption information are also included along with ascii listings of spectral reflectance for each sample. X-ray diffraction data for a limited set of the 52 expanded vermiculite samples are also given in figures included in the sample description pdf files. Scanning Electron micrographs of the expanded vermiculite samples or their sink fractions are also presented in the sample description pdf files. Some of these samples, particularly the ones from Libby, Montana contain bundles of elongate amphibole capable of causing asbestosis, lung cancer, and mesothelioma. This release encompasses all of the data used to support the journal publication and can be more fully understood when referring to that publication.