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The unique capabilities of ultrashort pulse femtosecond lasers have been integrated with a focused ion beam (FIB) platform to create a new system for rapid 3D materials analysis. The femtosecond laser allows for in situ layer-by-layer material ablation with high material removal rates. The high pulse frequency (1 kHz) of ultrashort (150 fs) laser pulses can induce material ablation with virtually no thermal damage to the surrounding area, permitting high resolution imaging, as well as crystallographic and elemental analysis, without intermediate surface preparation or removal of the sample from the chamber. The TriBeam system combines the high resolution and broad detector capabilities of the DualBeam(TM) microscope with the high material removal rates of the femtosecond laser, allowing 3D datasets to be acquired at rates 4-6 orders of magnitude faster than 3D FIB datasets. Design features that permit coupling of laser and electron optics systems and positioning of a stage in the multiple analysis positions are discussed. Initial in situ multilayer data are presented.