Ultrafast electron microscopy and diffraction are powerful techniques for the study of the time-resolved structures of molecules, materials, and biological systems. Central to these approaches is the use of ultrafast coherent electron packets. The electron pulses typically have an energy of 30 keV for diffraction and 100 -200 keV for microscopy, corresponding to speeds of 33-70% of the speed of light. Although the spatial resolution can reach the atomic scale, the temporal resolution is limited by the pulse width and by the difference in group velocities of electrons and the light used to initiate the dynamical change. In this contribution, we introduce the concept of tilted optical pulses into diffraction and imaging techniques and demonstrate the methodology experimentally. These advances allow us to reach limits of time resolution down to regimes of a few femtoseconds and, possibly, attoseconds. With tilted pulses, every part of the sample is excited at precisely the same time as when the electrons arrive at the specimen. Here, this approach is demonstrated for the most unfavorable case of ultrafast crystallography. We also present a method for measuring the duration of electron packets by autocorrelating electron pulses in free space and without streaking, and we discuss the potential of tilting the electron pulses themselves for applications in domains involving nuclear and electron motions.ultrafast imaging ͉ femtosecond electron pulses ͉ electron autocorrelation I n recent years it has become possible to reveal structures and dynamics with combined atomic-scale spatial and temporal resolutions in the gas phase, on surfaces and in crystals, and for biological systems, by using 4D ultrafast electron diffraction, crystallography, and microscopy (ref. 1 and references therein). The spatial resolution in ultrafast electron diffraction is atomic with milliangstrom accuracy, and the temporal resolution is up to subpicosecond at low electron fluxes (ref. 2 and references therein; see also refs. 3 and 4), well suited to resolve ultrafast dynamics. The temporal limit is determined by the extent of energy spread and space charge effects (ref. 5 and references therein). Recently, by developing microscopy and diffraction with single-electron packets (6), space charge effects and their associated pulse broadening mechanisms were fully removed, reaching the femtosecond regime for imaging with electrons. For reversible processes, an ultrafast dynamics can be measured with pulse trains at high repetition rates. However, for irreversible changes, a single pulse must have such a large number of electrons that the temporal broadening has to be considered at the point of in situ imaging.Besides the pulse duration, there is another temporal spread that imposes an often more severe limitation on time resolution. When performing experiments with pulses of different speed, such as the case here for electrons and photons (used to initiate the change), one has to consider the different group velocities involved. For electrons accel...