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In this paper, we reported the application of TEM‐based techniques for the physical characterization and failure analysis of OLED devices. By using our new FIB‐TEM techniques, we successfully identified nanoscale multilayered organic film stacks in OLED devices, enabling the failure root understanding of the dark emission of R pixels in an OLD device. Other two case studies presented in this work demonstrated the importance of the combination of plane‐view FIB‐TEM with cross‐section FIB‐TEM techniques, and the grain size analysis techniques by TEM for the failure analysis of the OLED devices.