The Far-Infrared Radiation Mobile Observation System (FIRMOS) is a Fourier transform spectroradiometer developed to support the Far-infrared Outgoing Radiation Understanding and Monitoring (FORUM) satellite mission by validating measurement methods and instrument design concepts, both in the laboratory and in field campaigns. FIRMOS is capable of measuring the downwelling spectral radiance emitted by the atmosphere in the spectral band from 100 to 1000 cm−1 (10–100 µm in wavelength), with a maximum spectral resolution of 0.25 cm−1. We describe the instrument design and its characterization and discuss the geophysical products obtained by inverting the atmospheric spectral radiance measured during a campaign from the high-altitude location of Mount Zugspitze in Germany, beside the Extended-range Atmospheric Emitted Radiance Interferometer (E-AERI), which is permanently installed at the site. Following the selection of clear-sky scenes, using a specific algorithm, the water vapour and temperature profiles were retrieved from the FIRMOS spectra by applying the Kyoto protocol and Informed Management of the Adaptation (KLIMA) code. The profiles were found in very good agreement with those provided by radiosondes and by the Raman lidar operating from the Zugspitze Schneefernerhaus station. In addition, the retrieval products were validated by comparing the retrieved integrated water vapour values with those obtained from the E-AERI spectra.