This dataset contains reflectance and transmission spectra of unexpanded and expanded vermiculite ore, and handpicked flakes of phlogopite, hydrobiotite, and vermiculite. These samples were collected from mines near Enoree, South Carolina; Libby, Montana; Louisa, Virginia; Palabora, Llano, Texas; and South Africa. Spectra are identified as either reflectance or transmission in the alphanumeric file names and correlate to specpr record numbers designated in the manuscript figures in which they are shown. These transmission spectra were converted to absorbance in many of the figures. Spectra of talc, fibrous richterite amphibole, and serpentine are from well characterized samples from Feiser Mine, Ruby Mountains, Montana; Libby, Montana; and a NIOSH chrysotile standard (CH29) respectively. The talc sample is described in the U.S. Geological Survey Spectral Library (Kokaly and others, 2017). Some vermiculite samples were K-exchanged to facilitate spectral comparisons.