Femtosecond laser ablation offers the unique ability to remove material at rates that are orders of magnitude faster than existing ion beam technologies with little or no associated damage. By combining ultrafast lasers with state-of-the-art electron microscopy equipment, we have developed a TriBeam system capable of targeted, in-situ tomography providing chemical, structural, and topographical information in three dimensions of near mm³ sized volumes. The origins, development, physics, current uses, and future potential for the TriBeam system are described in this tutorial review.