Radiation detectors monitored trains at two international borders to evaluate the performance of NaI(Tl) and plastic (polyvinyltoluene: PVT) gamma-ray detectors to characterize rail cargo. The detectors included a prototype NaI(Tl) radiation-portal-monitor panel having four large detectors (10-cm × 10-cm × 41-cm) and a PVT panel with a 41 cm × 173 cm × 3.8-cm detector. Spectral data from the NaI(Tl) and PVT detectors were recorded. Of particular emphasis was the identification of naturally occurring radioactive material (NORM) and the resultant frequency of nuisance alarms. For rail monitoring, the difficulty in stopping trains to perform secondary inspection on alarming cars creates a need for reliable identification of NORM during initial screening. Approximately 30 trains were monitored, and the commodities in individual railcars were ascertained from manifest information. At one test site, the trains carried inter-modal containers that had been unloaded from ships, and at the other site, the trains contained bulk cargo in tanker cars and hopper cars or individual items in boxcars or flatbeds. NORM encountered included potash, liquefied petroleum gas, fireworks, televisions, and clay-based products (e.g., pottery). Analysis of the spectral data included the use of the template-fitting portion of the program GADRAS developed at Sandia National Laboratories. For most of the NORM, the NaI(Tl) data produced a correct identification of the radionuclides present in the railcars. The same analysis was also used for PVT data in which the spectral information (no peaks but only gradual spectral changes including Compton edges) was limited. However, the PVT analysis provided correct identification of 40K and 226Ra in many cases.