We are currently developing high-resolution high-efficiency microcolumnar LiI films for thermal neutron imaging. The films are produced by the vapor deposition of LiI on a fiber-optic substrate and hermetically sealed in a specially designed aluminum package. Our work has produced up to 1.2-mm-thick films with column diameters of approximately 30 m. We have also performed imaging studies by optically coupling some of these films to a fiber-optic taper-based charge-coupled device. The imaging performance of the system was experimentally evaluated at Radiation Monitoring Devices, Inc., as well as at the thermal neutron port of the University of Massachusetts Lowell Research Reactor. The LiI films exhibited excellent scintillation characteristics with a spatial resolution as high as 4.5 lp/mm (line pairs per millimeter). This paper outlines the film characterization and performance evaluation conducted during the course of the study. The new sensor described here is expected to usher in the development of large-area high-resolution digital thermal neutron detectors with improved detection efficiency and dynamic range and faster readout times than the current sensors.Index Terms-Digital neutron imaging, neutron radiography, structured scintillator, thermal neutron imaging.