At 75, gas-phase electron diffraction is still the method of choice for selected problems in molecular structure determination. It works best when being applied with other techniques in a concerted way.KEY WORDS: Gas-phase electron diffraction; molecular structure.The first paper describing gas-phase electron diffraction appeared in 1930; its authors were Herman F. Mark and Raimund Wierl [1]. Mark was a chemist who later became famous for his pioneering polymer studies and Wierl was a physicist, who died young. The origins of the new technique for the determination of molecular structure go back to the 1910s and 20s. Peter Debye as early as 1915 demonstrated that X-rays scattered by a gaseous sample of carbon tetrachloride formed a diffraction pattern [2]. Then Louis de Broglie concluded the wave-particle duality of fast-moving particles, and the experimental verification on solids was given by Davisson and Germer for slow electrons [3] and by Thomson for fast electrons [4]. The very first gas-phase electron diffraction experiment [1] was carried out on carbon tetrachloride vapor; it used 45-kV electrons and an exposure time of a tenth of a second! In a straightforward way, Mark and Wierl determined the C Cl interatomic distance from the electron diffraction pattern, which was orders of magnitude quicker to produce, and it was less diffuse and of higher contrast than the X-ray diffraction patterns [5].A new technique for molecular structure determination was born, which has been around ever since. From 1930, it has played an important role in accumulating structural data and in developing qualitative and quantitative models and theories of structure and bonding. Numerous references to electron diffraction struc-