In high-temperature cuprate superconductors, it is now generally agreed that superconductivity is realized by doping an antiferromagnetic Mott (charge transfer) insulator. The doping-induced insulator-to-superconductor transition has been widely observed in cuprates, which provides important information for understanding the superconductivity mechanism. In the iron-based superconductors, however, the parent compound is mostly antiferromagnetic bad metal, raising a debate on whether an appropriate starting point should go with an itinerant picture or a localized picture. No evidence of doping-induced insulator-superconductor transition (or crossover) has been reported in the iron-based compounds so far. Here, we report an electronic evidence of an insulator-superconductor crossover observed in the single-layer FeSe film grown on a SrTiO 3 substrate. By taking angle-resolved photoemission measurements on the electronic structure and energy gap, we have identified a clear evolution of an insulator to a superconductor with increasing carrier concentration. In particular, the insulator-superconductor crossover in FeSe/SrTiO 3 film exhibits similar behaviors to that observed in the cuprate superconductors. Our results suggest that the observed insulator-superconductor crossover may be associated with the twodimensionality that enhances electron localization or correlation. The reduced dimensionality and the interfacial effect provide a new pathway in searching for new phenomena and novel superconductors with a high transition temperature.single-layer FeSe/SrTiO 3 films | insulator-to-superconductor crossover | ARPES T he iron-based superconductors (1-4) represent the second class of high-temperature superconductors after the discovery of the first class of high-temperature cuprate superconductors. It is now generally agreed that the superconductivity in cuprates is realized by doping a Mott (charge transfer) insulator (5). In the iron-based superconductors, however, the parent compounds mostly exhibit a poor metallic behavior with an antiferromagnetic order, thus raising a debate on whether an appropriate starting point should go with an itinerant picture or a localized picture (6-18), particularly whether the picture of doping a Mott insulator is relevant to the iron-based superconductors (1,3,11,16,17). Some theoretical calculations indicate that the iron-based superconductors may be in proximity to a Mott insulator (11,16,17), and attempts have also been made to unify cuprates and ironbased superconductors in theory (18). However, so far no clear experimental evidence of doping (or carrier concentration)-induced insulator-superconductor transition (or crossover) has been reported in the iron-based superconductors.The latest discovery of possible high-temperature superconductivity in the single-layer FeSe films grown on a SrTiO 3 substrate has attracted much attention both experimentally (19)(20)(21)(22)(23)(24)(25)(26)(27) and theoretically (28-32). The reduced dimensionality with enhanced interfacial effect makes ...