The Bagnold linear dune field investigated by Curiosity at Mount Desert Island (MDI) is to the north of the ~5.5 km high Aeolis Mons mound in Gale crater. False-color images (RGB, 2.496, 1.802, and 1.235 µm, respectively) generated from Mars Reconnaissance Orbiter (MRO) Compact Reconnaissance Imaging Spectrometer for Mars (CRISM) data show the dune field has a reddish-brown color. The Sands of Forvie (SoF), located ~2.5 km to the southeast of MDI, is darker and lacks the reddish-brown color. Single scattering albedo (SSA) spectra retrieved at 12 m/pixel using along‑track oversampled CRISM observation FRT00021C92 show a long wavelength (1.7 to 2.5 µm) increase in albedo for MDI dunes. For the same interval, SoF is characterized by a broad ~2.2 µm absorption feature, consistent with color differences between the two deposits. Checkerboard un-mixing of the SSA image cube was used to isolate spectral endmembers within the MDI and SoF deposits. Radiative modeling of the CRISM endmember spectra using Hapke (2012) theory implies finer grain sizes for MDI as compared to SoF, with more pigeonite, plagioclase, and olivine, and less basaltic glass and augite as compared to SoF deposit. These results are consistent with Curiosity‑based observations that MDI contains smaller ripples with overall finer grains, whereas SoF has large ripples and coarser grains on their crests. Although these deposits are only located ~2.5 kilometers away from one another, wind and local topographic controls are interpreted to have modulated grain sizes and mineralogy. This dataset contains the hyperspectral image cubes that were processed for use in this study, regions of interest (ROI) data for SoF and MDI as described above, and spectra of the synthesized glass endmembers used for spectral modeling.