Atom probe tomography (APT) data acquired from a CAMECA LEAP 4000 XHR for the CdS/CdTe interface for a non-CdCl2 treated CdTe solar cell as well as the mass spectrum of an APT data set including a GB in a CdCl2-treated CdTe solar cell are presented. Scanning electron microscopy (SEM) data showing the evolution of sample preparation for APT and scanning transmission electron microscopy (STEM) electron beam induced current (EBIC) are also presented. These data show mass spectrometry peak decomposition of Cu and Te within an APT dataset, the CdS/CdTe interface of an untreated CdTe solar cell, preparation of APT needles from the CdS/CdTe interface in superstrate grown CdTe solar cells, and the preparation of a cross-sectional STEM EBIC sample.