Atomic-scale control and manipulation of the microstructure of polycrystalline thin films during kinetically limited low-temperature deposition, crucial for a broad range of industrial applications, has been a leading goal of materials science during the past decades. Here, we review the present understanding of film growth processes—nucleation, coalescence, competitive grain growth, and recrystallization—and their role in microstructural evolution as a function of deposition variables including temperature, the presence of reactive species, and the use of low-energy ion irradiation during growth.