Atomic layer epitaxy (ALE) is not so much a new technique for the preparation of thin films as a novel modification to existing methods of vapor‐phase epitaxy, whether physical [e.g., evaporation, at one limit molecular‐beam epitaxy (MBE)] or chemical [e.g., chloride epitaxy or metalorganic chemical vapor deposition (MOCVD)]. It is a self‐regulatory process which, in its simplest form, produces one complete molecular layer of a compound per operational cycle, with a greater thickness being obtained by repeated cycling. There is no growth rate in ALE as in other crystal growth processes. So far ALE has been applied to rather few materials, but, in principle, it could have a quite general application. It has been used to prepare single‐crystal overlayers of CdTe, (Cd,Mn)Te, GaAs and AlAs, a number of polycrystalline films and highly efficient electroluminescent thin‐film displays based on ZnS:Mn. It could also offer particular advantages for the preparation of ultrathin films of precisely controlled thickness in the nanometer range and thus may have a special value for growing low‐dimensional structures.