Optical microbunches with a spacing of 800 nm have been produced for laser acceleration research. The microbunches are produced using a inverse Free-Electron-Laser (IFEL) followed by a dispersive chicane. The microbunched electron beam is characterized by coherent optical transition radiation (COTR) with good agreement to the analytic theory for bunch formation. In a second experiment the bunches are accelerated in a second stage to achieve for the first time direct net acceleration of electrons traveling in a vacuum with visible light. This dissertation presents the theory of microbunch formation and characterization of the microbunches. It also presents the design of the experimental hardware from magnetostatic and particle tracking simulations, to fabrication and measurement of the undulator and chicane magnets. Finally, the dissertation discusses three experiments aimed at demonstrating the IFEL interaction, microbunch production, and the net acceleration of the microbunched beam. At the close of the dissertation, a separate but related research effort on the tight focusing of electrons for coupling into optical scale, Photonic Bandgap, structures is presented. This includes the design and fabrication of a strong focusing permanent magnet quadrupole triplet and an outline of an initial experiment using the triplet to observe wakefields generated by an electron …