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The data are nanoindentation, high-angular resolution electron backscatter diffraction (HR-EBSD), and transmission electron microscopy data collected on samples of synthetic forsterite bicrystals at room temperature. The data were collected in two samples, with high- and low- angle grain boundaries (HAGB, 60°, [100]/(011) and SB, 13°, [100]/(016)). The EBSD data are the basis for the HR-EBSD calculation. The HR-EBSD results are presented as Matlab data files. The nanoindentation data are categorised as a function of sample (‘ol13’ – low-angle grain boundary; and ‘ol60’ – high-angle grain boundary), and indenter tip geometry (spherical (with a 10 or 5 micron radius) and pyramidal (Berkovich). The data are presented in .xls files. The TEM data are presented as .tif files. The TEM data were collected in specific indents with various distances from the interfaces. These data have been published in the manuscript: : The Role of Grain Boundaries in Low-Temperature Plasticity of Olivine Revealed by Nanoindentation, with the DOI: 10.1029/2023JB026763