This dataset provides the raw data to the manuscript "Link between Anisotropic Electrochemistry and Surface Transformations at Single Crystal Silicon Electrodes: Implications for Lithium Ion Batteries" Specifically, the following measurements are provided: Electrochemical measurements as cyclic voltammetry using scanning electrochemical cell microscopy for three different Si crystallographic orientations (100, 110, 311) in 1 M LiPF6 in ethylene carbonate - ethyl methyl carbonate ("SECCM/") Scanning electron microscopy and transmission electron microscopy imaging of pristine and cycled samples ("Images/")